Hongjie Dai

All Publications

• A human autoimmune organoid model reveals IL-7 function in coeliac disease. Nature Santos, A. J., van Unen, V., Lin, Z., Chirieleison, S. M., Ha, N., Batish, A., Chan, J. E., Cedano, J., Zhang, E. T., Mu, Q., Guh-Siesel, A., Tomaske, M., Colburg, D., Varma, S., Choi, S. S., Christophersen, A., Baghdasaryan, A., Yost, K. E., Karlsson, K., Ha, A., Li, J., Dai, H., Sellers, Z. M., Chang, H. Y., Dunn, J. C., Zhang, B. M., Mellins, E. D., Sollid, L. M., Fernandez-Becker, N. Q., Davis, M. M., Kuo, C. J. 2024

  Abstract

  In vitro models of autoimmunity are constrained by an inability to culture affected epithelium alongside the complex tissue-resident immune microenvironment. Coeliac disease (CeD) is an autoimmune disease in which dietary gluten-derived peptides bind to the major histocompatibility complex (MHC) class II human leukocyte antigen molecules (HLA)-DQ2 or HLA-DQ8 to initiate immune-mediated duodenal mucosal injury1-4. Here, we generated air-liquid interface (ALI) duodenal organoids from intact fragments of endoscopic biopsies that preserve epithelium alongside native mesenchyme and tissue-resident immune cells as a unit without requiring reconstitution. The immune diversity of ALI organoids spanned T cells, B and plasma cells, natural killer (NK) cells and myeloid cells, with extensive T-cell and B-cell receptor repertoires. HLA-DQ2.5-restricted gluten peptides selectively instigated epithelial destruction in HLA-DQ2.5-expressing organoids derived from CeD patients, and this was antagonized by blocking MHC-II or NKG2C/D. Gluten epitopes stimulated a CeD organoid immune network response in lymphoid and myeloid subsets alongside anti-transglutaminase 2 (TG2) autoantibody production. Functional studies in CeD organoids revealed that interleukin-7 (IL-7) is a gluten-inducible pathogenic modulator that regulates CD8+ T-cell NKG2C/D expression and is necessary and sufficient for epithelial destruction. Furthermore, endogenous IL-7 was markedly upregulated in patient biopsies from active CeD compared with remission disease from gluten-free diets, predominantly in lamina propria mesenchyme. By preserving the epithelium alongside diverse immune populations, this human in vitro CeD model recapitulates gluten-dependent pathology, enables mechanistic investigation and establishes a proof of principle for the organoid modelling of autoimmunity.

  View details for DOI 10.1038/s41586-024-07716-2

  View details for PubMedID 39048815

• In vivo NIR-II fluorescence imaging for biology and medicine NATURE PHOTONICS Wang, F., Zhong, Y., Bruns, O., Liang, Y., Dai, H. 2024

  View details for DOI 10.1038/s41566-024-01391-5

  View details for Web of Science ID 001178071900001

• Analysis of Si, Cu, and Their Oxides by X-ray Photoelectron Spectroscopy JOURNAL OF CHEMICAL EDUCATION Li, J., Zhu, G., Liang, P., Dai, H. 2024; 101 (3): 1162-1170

  View details for DOI 10.1021/acs.jchemed.3c00848

  View details for Web of Science ID 001174400400001

• Intratumor injected gold molecular clusters for NIR-II imaging and cancer therapy. Proceedings of the National Academy of Sciences of the United States of America Baghdasaryan, A., Liu, H., Ren, F., Hsu, R., Jiang, Y., Wang, F., Zhang, M., Grigoryan, L., Dai, H. 2024; 121 (5): e2318265121

  Abstract

  Surgical resections of solid tumors guided by visual inspection of tumor margins have been performed for over a century to treat cancer. Near-infrared (NIR) fluorescence labeling/imaging of tumor in the NIR-I (800 to 900 nm) range with systemically administrated fluorophore/tumor-targeting antibody conjugates have been introduced to improve tumor margin delineation, tumor removal accuracy, and patient survival. Here, we show Au25 molecular clusters functionalized with phosphorylcholine ligands (AuPC, ~2 nm in size) as a preclinical intratumorally injectable agent for NIR-II/SWIR (1,000 to 3,000 nm) fluorescence imaging-guided tumor resection. The AuPC clusters were found to be uniformly distributed in the 4T1 murine breast cancer tumor upon intratumor (i.t.) injection. The phosphocholine coating afforded highly stealth clusters, allowing a high percentage of AuPC to fill the tumor interstitial fluid space homogeneously. Intra-operative surgical navigation guided by imaging of the NIR-II fluorescence of AuPC allowed for complete and non-excessive tumor resection. The AuPC in tumors were also employed as a photothermal therapy (PTT) agent to uniformly heat up and eradicate tumors. Further, we performed in vivo NIR-IIb (1,500 to 1,700 nm) molecular imaging of the treated tumor using a quantum dot-Annexin V (QD-P3-Anx V) conjugate, revealing cancer cell apoptosis following PTT. The therapeutic functionalities of AuPC clusters combined with rapid renal excretion, high biocompatibility, and safety make them promising for clinical translation.

  View details for DOI 10.1073/pnas.2318265121

  View details for PubMedID 38261618

• Electrochemical acetate production from high-pressure gaseous and liquid CO₂ NATURE CATALYSIS Li, J., Kuang, Y., Zhang, X., Hung, W., Chiang, C., Zhu, G., Chen, G., Wang, F., Liang, P., Dai, H. 2023

  View details for DOI 10.1038/s41929-023-01046-8

  View details for Web of Science ID 001085944100001

• Rechargeable Li/Cl2 Battery Down to -80 °C. Advanced materials (Deerfield Beach, Fla.) Liang, P., Zhu, G., Huang, C. L., Li, Y. Y., Sun, H., Yuan, B., Wu, S. C., Li, J., Wang, F., Hwang, B. J., Dai, H. 2023: e2307192

  Abstract

  Low temperature rechargeable batteries are important to life in cold climates, polar/deep-sea expeditions and space explorations. Here, we report 3.5 - 4 V rechargeable lithium/chlorine (Li/Cl2 ) batteries operating down to -80°C, employing Li metal negative electrode, a novel CO2 activated porous carbon (KJCO2 ) as the positive electrode, and a high ionic conductivity (∼ 5 to 20 mS cm-1 from -80°C to room-temperature) electrolyte comprised of aluminum chloride (AlCl3 ), lithium chloride (LiCl), and lithium bis(fluorosulfonyl)imide (LiFSI) in low-melting-point (-104.5 °C) thionyl chloride (SOCl2 ). Between room-temperature and -80°C, the Li/Cl2 battery delivered up to ∼ 29,100 - 4,500 mAh g-1 first discharge capacity (based on carbon mass) and a 1,200 - 5,000 mAh g-1 reversible capacity over up to 130 charge-discharge cycles. Mass spectrometry and X-ray photoelectron spectroscopy probed Cl2 trapped in the porous carbon upon LiCl electro-oxidation during charging. At -80°C, Cl2 /SCl2 /S2 Cl2 generated by electro-oxidation in the charging step were trapped in porous KJCO2 carbon, allowing for reversible reduction to afford a high discharge voltage plateau near ∼ 4 V with up to ∼ 1000 mAh g-1 capacity for SCl2 /S2 Cl2 reduction and up to ∼ 4000 mAh g-1 capacity at ∼ 3.1 V plateau for Cl2 reduction. This article is protected by copyright. All rights reserved.

  View details for DOI 10.1002/adma.202307192

  View details for PubMedID 37804146

• Shedding light on rechargeable Na/Cl2 battery. Proceedings of the National Academy of Sciences of the United States of America Zhu, G., Liang, P., Huang, C. L., Wu, S. C., Huang, C. C., Li, Y. Y., Jiang, S. K., Huang, W. H., Li, J., Wang, F., Hwang, B. J., Dai, H. 2023; 120 (39): e2310903120

  Abstract

  Advancing new ideas of rechargeable batteries represents an important path to meeting the ever-increasing energy storage needs. Recently, we showed rechargeable sodium/chlorine (Na/Cl2) (or lithium/chlorine Li/Cl2) batteries that used a Na (or Li) metal negative electrode, a microporous amorphous carbon nanosphere (aCNS) positive electrode, and an electrolyte containing dissolved aluminum chloride and fluoride additives in thionyl chloride [G. Zhu et al., Nature 596, 525-530 (2021) and G. Zhu et al., J. Am. Chem. Soc. 144, 22505-22513 (2022)]. The main battery redox reaction involved conversion between NaCl and Cl2 trapped in the carbon positive electrode, delivering a cyclable capacity of up to 1,200 mAh g-1 (based on positive electrode mass) at a ~3.5 V discharge voltage [G. Zhu et al., Nature 596, 525-530 (2021) and G. Zhu et al., J. Am. Chem. Soc. 144, 22505-22513 (2022)]. Here, we identified by X-ray photoelectron spectroscopy (XPS) that upon charging a Na/Cl2 battery, chlorination of carbon in the positive electrode occurred to form carbon-chlorine (C-Cl) accompanied by molecular Cl2 infiltrating the porous aCNS, consistent with Cl2 probed by mass spectrometry. Synchrotron X-ray diffraction observed the development of graphitic ordering in the initially amorphous aCNS under battery charging when the carbon matrix was oxidized/chlorinated and infiltrated with Cl2. The C-Cl, Cl2 species and graphitic ordering were reversible upon discharge, accompanied by NaCl formation. The results revealed redox conversion between NaCl and Cl2, reversible graphitic ordering/amorphourization of carbon through battery charge/discharge, and probed trapped Cl2 in porous carbon by XPS.

  View details for DOI 10.1073/pnas.2310903120

  View details for PubMedID 37729201

• Multiplexed discrimination of SARS-CoV-2 variants via plasmonic-enhanced fluorescence in a portable and automated device. Nature biomedical engineering Liu, Y., Yang, Y., Wang, G., Wang, D., Shao, P., Tang, J., He, T., Zheng, J., Hu, R., Liu, Y., Xu, Z., Niu, D., Lv, J., Yang, J., Xiao, H., Wu, S., He, S., Tang, Z., Liu, Y., Tang, M., Jiang, X., Yuan, J., Dai, H., Zhang, B. 2023

  Abstract

  Portable assays for the rapid identification of lineages of severe acute respiratory syndrome coronavirus 2 (SARS-CoV-2) are needed to aid large-scale efforts in monitoring the evolution of the virus. Here we report a multiplexed assay in a microarray format for the detection, via isothermal amplification and plasmonic-gold-enhanced near-infrared fluorescence, of variants of SARS-CoV-2. The assay, which has single-nucleotide specificity for variant discrimination, single-RNA-copy sensitivity and does not require RNA extraction, discriminated 12 lineages of SARS-CoV-2 (in three mutational hotspots of the Spike protein) and detected the virus in nasopharyngeal swabs from 1,034 individuals at 98.8% sensitivity and 100% specificity, with 97.6% concordance with genome sequencing in variant discrimination. We also report a compact, portable and fully automated device integrating the entire swab-to-result workflow and amenable to the point-of-care detection of SARS-CoV-2 variants. Portable, rapid, accurate and multiplexed assays for the detection of SARS-CoV-2 variants and lineages may facilitate variant-surveillance efforts.

  View details for DOI 10.1038/s41551-023-01092-4

  View details for PubMedID 37735541

• Shortwave-infrared-light-emitting probes for the in vivo tracking of cancer vaccines and the elicited immune responses. Nature biomedical engineering Ren, F., Wang, F., Baghdasaryan, A., Li, Y., Liu, H., Hsu, R., Wang, C., Li, J., Zhong, Y., Salazar, F., Xu, C., Jiang, Y., Ma, Z., Zhu, G., Zhao, X., Wong, K. K., Willis, R., Christopher Garcia, K., Wu, A., Mellins, E., Dai, H. 2023

  Abstract

  Tracking and imaging immune cells in vivo non-invasively would offer insights into the immune responses induced by vaccination. Here we report a cancer vaccine consisting of polymer-coated NaErF4/NaYF4 core-shell down-conversion nanoparticles emitting luminescence in the near-infrared spectral window IIb (1,500-1,700 nm in wavelength) and with surface-conjugated antigen (ovalbumin) and electrostatically complexed adjuvant (class-B cytosine-phosphate-guanine). Whole-body wide-field imaging of the subcutaneously injected vaccine in tumour-bearing mice revealed rapid migration of the nanoparticles to lymph nodes through lymphatic vessels, with two doses of the vaccine leading to the complete eradication of pre-existing tumours and to the prophylactic inhibition of tumour growth. The abundance of antigen-specific CD8+ T lymphocytes in the tumour microenvironment correlated with vaccine efficacy, as we show via continuous-wave imaging and lifetime imaging of two intravenously injected near-infrared-emitting probes (CD8+-T-cell-targeted NaYbF4/NaYF4 nanoparticles and H-2Kb/ovalbumin257-264 tetramer/PbS/CdS quantum dots) excited at different wavelengths, and by volumetrically visualizing the three nanoparticles via light-sheet microscopy with structured illumination. Nanoparticle-based vaccines and imaging probes emitting infrared light may facilitate the design and optimization of immunotherapies.

  View details for DOI 10.1038/s41551-023-01083-5

  View details for PubMedID 37620621

  View details for PubMedCentralID 7157724

• Seeing into deep tissue NATURE PHOTONICS Pitruzzello, G., Dai Hongjie 2023

  View details for DOI 10.1038/s41566-023-01200-5

  View details for Web of Science ID 000970902100001

• High-Capacity Rechargeable Li/Cl2 Batteries with Graphite Positive Electrodes. Journal of the American Chemical Society Zhu, G., Liang, P., Huang, C. L., Huang, C. C., Li, Y. Y., Wu, S. C., Li, J., Wang, F., Tian, X., Huang, W. H., Jiang, S. K., Hung, W. H., Chen, H., Lin, M. C., Hwang, B. J., Dai, H. 2022

  Abstract

  Developing new types of high-capacity and high-energy density rechargeable batteries is important to future generations of consumer electronics, electric vehicles, and mass energy storage applications. Recently, we reported ∼3.5 V sodium/chlorine (Na/Cl2) and lithium/chlorine (Li/Cl2) batteries with up to 1200 mAh g-1 reversible capacity, using either a Na or a Li metal as the negative electrode, an amorphous carbon nanosphere (aCNS) as the positive electrode, and aluminum chloride (AlCl3) dissolved in thionyl chloride (SOCl2) with fluoride-based additives as the electrolyte [Zhu et al., Nature, 2021, 596 (7873), 525-530]. The high surface area and large pore volume of aCNS in the positive electrode facilitated NaCl or LiCl deposition and trapping of Cl2 for reversible NaCl/Cl2 or LiCl/Cl2 redox reactions and battery discharge/charge cycling. Here, we report an initially low surface area/porosity graphite (DGr) material as the positive electrode in a Li/Cl2 battery, attaining high battery performance after activation in carbon dioxide (CO2) at 1000 °C (DGr_ac) with the first discharge capacity ∼1910 mAh g-1 and a cycling capacity up to 1200 mAh g-1. Ex situ Raman spectroscopy and X-ray diffraction (XRD) revealed the evolution of graphite over battery cycling, including intercalation/deintercalation and exfoliation that generated sufficient pores for hosting LiCl/Cl2 redox. This work opens up widely available, low-cost graphitic materials for high-capacity alkali metal/Cl2 batteries. Lastly, we employed mass spectrometry to probe the Cl2 trapped in the graphitic positive electrode, shedding light into the Li/Cl2 battery operation.

  View details for DOI 10.1021/jacs.2c07826

  View details for PubMedID 36450002

• Structural engineering of alpha-MnO2 cathode by Ag plus incorporation for high capacity aqueous zinc-ion batteries JOURNAL OF POWER SOURCES Fenta, F., Olbasa, B., Tsai, M., Temesgen, N., Huang, W., Tekaligne, T., Nikodimos, Y., Wu, S., Su, W., Dai, H., Hwang, B. 2022; 548

  View details for DOI 10.1016/j.jpowsour.2022.232010

  View details for Web of Science ID 000863224900002

• A Non-Flammable High-Voltage 4.7 V Anode-Free Lithium Battery. Advanced materials (Deerfield Beach, Fla.) Liang, P., Sun, H., Huang, C., Zhu, G., Tai, H., Li, J., Wang, F., Wang, Y., Huang, C., Jiang, S., Lin, M., Li, Y., Hwang, B., Wang, C., Dai, H. 2022: e2207361

  Abstract

  Anode-free lithium metal batteries employ in-situ lithium plated current collectors as negative electrodes to afford optimal mass and volumetric energy densities. The main challenges to such batteries include their poor cycling stability and safety issues of flammable organic electrolytes. Here, we report a high-voltage 4.7V anode-free lithium metal battery using a Cu foil coated with a layer ( 950nm) of silicon-polyacrylonitrile (Si-PAN, 25.5mug cm-2 ) as the negative electrode, a high-voltage cobalt-free LiNi0.5 Mn1.5 O4 (LNMO) as the positive electrode and a safe, non-flammable ionic liquid electrolyte comprised of 4.5M lithium bis(fluorosulfonyl)imide (LiFSI) salt in N-methyl-N-propyl pyrrolidiniumbis(fluorosulfonyl)imide (Py13 FSI) with 1 wt% lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) as additive. The Si-PAN coating was found to seed the growth of lithium during charging, and reversibly expand/shrink during lithium plating/stripping over battery cycling. The wide voltage-window electrolyte containing a high concentration of FSI- and TFSI- facilitated the formation of stable solid-electrolyte interphase, affording a 4.7V anode-free Cu@Si-PAN/LiNi0.5 Mn1.5 O4 battery with a reversible specific capacity of 120 mAh g-1 and high cycling stability (80% capacity retention after 120 cycles). These results represent the first anode-free Li battery with a high 4.7V discharge voltage and high safety. This article is protected by copyright. All rights reserved.

  View details for DOI 10.1002/adma.202207361

  View details for PubMedID 36193778

• Phosphorylcholine-conjugated gold-molecular clusters improve signal for Lymph Node NIR-II fluorescence imaging in preclinical cancer models. Nature communications Baghdasaryan, A., Wang, F., Ren, F., Ma, Z., Li, J., Zhou, X., Grigoryan, L., Xu, C., Dai, H. 2022; 13 (1): 5613

  Abstract

  Sentinel lymph node imaging and biopsy is important to clinical assessment of cancer metastasis, and novel non-radioactive lymphographic tracers have been actively pursued over the years. Here, we develop gold molecular clusters (Au25) functionalized by phosphorylcholine (PC) ligands for NIR-II (1000-3000nm) fluorescence imaging of draining lymph nodes in 4T1 murine breast cancer and CT26 colon cancer tumor mouse models. The Au-phosphorylcholine (Au-PC) probes exhibit 'super-stealth' behavior with little interactions with serum proteins, cells and tissues in vivo, which differs from the indocyanine green (ICG) dye. Subcutaneous injection of Au-PC allows lymph node mapping by NIR-II fluorescence imaging at an optimal time of ~ 0.5 - 1hour postinjection followed by rapid renal clearance. Preclinical NIR-II fluorescence LN imaging with Au-PC affords high signal to background ratios and high safety and biocompatibility, promising for future clinical translation.

  View details for DOI 10.1038/s41467-022-33341-6

  View details for PubMedID 36153336

• In vivo non-invasive confocal fluorescence imaging beyond 1,700 nm using superconducting nanowire single-photon detectors. Nature nanotechnology Wang, F., Ren, F., Ma, Z., Qu, L., Gourgues, R., Xu, C., Baghdasaryan, A., Li, J., Zadeh, I. E., Los, J. W., Fognini, A., Qin-Dregely, J., Dai, H. 2022

  Abstract

  Light scattering by biological tissues sets a limit to the penetration depth of high-resolution optical microscopy imaging of live mammals in vivo. An effective approach to reduce light scattering and increase imaging depth is to extend the excitation and emission wavelengths to the second near-infrared window (NIR-II) at >1,000 nm, also called the short-wavelength infrared window. Here we show biocompatible core-shell lead sulfide/cadmium sulfide quantum dots emitting at ~1,880 nm and superconducting nanowire single-photon detectors for single-photon detection up to 2,000 nm, enabling a one-photon excitation fluorescence imaging window in the 1,700-2,000 nm (NIR-IIc) range with 1,650 nm excitation-the longest one-photon excitation and emission for in vivo mouse imaging so far. Confocal fluorescence imaging in NIR-IIc reached an imaging depth of ~1,100 μm through an intact mouse head, and enabled non-invasive cellular-resolution imaging in the inguinal lymph nodes of mice without any surgery. We achieve in vivo molecular imaging of high endothelial venules with diameters as small as ~6.6 μm, as well as CD169 + macrophages and CD3 + T cells in the lymph nodes, opening the possibility of non-invasive intravital imaging of immune trafficking in lymph nodes at the single-cell/vessel-level longitudinally.

  View details for DOI 10.1038/s41565-022-01130-3

  View details for PubMedID 35606441

• Probing dissolved CO2(aq) in aqueous solutions for CO2 electroreduction and storage. Science advances Li, J., Guo, J., Dai, H. 2022; 8 (19): eabo0399

  Abstract

  CO2 dissolved in aqueous solutions CO2(aq) is important to CO2 capture, storage, photo-/electroreduction in the fight against global warming and to CO2 analysis in drinks. Here, we developed microscale infrared (IR) spectroscopy for in situ dynamic quantitating CO2(aq). The quantized CO2(g) rotational state transitions were observed to quench for CO2(aq), accompanied by increased H2O IR absorption. An accurate CO2 molar extinction coefficient ε was derived for in situ CO2(aq) quantification up to 58 atm. We directly measured CO2(aq) concentrations in electrolytes under CO2(g) bubbling and high-pressure conditions with high spectral and time resolutions. In KHCO3 electrolytes with CO2(aq) > ~1 M, CO2 electroreduction (CO2RR) to formate reached >98% Faradaic efficiencies on copper (Cu2O/Cu)-based electrocatalyst. Furthermore, CO2 dissolution/desolvation kinetics showed large hysteresis and ultraslow reversal of CO2(aq) supersaturation in aqueous systems, with implications to CO2 capture, storage, and supersaturation phenomena in natural water bodies.

  View details for DOI 10.1126/sciadv.abo0399

  View details for PubMedID 35559679

• High-precision tumor resection down to few-cell level guided by NIR-IIb molecular fluorescence imaging. Proceedings of the National Academy of Sciences of the United States of America Wang, F., Qu, L., Ren, F., Baghdasaryan, A., Jiang, Y., Hsu, R., Liang, P., Li, J., Zhu, G., Ma, Z., Dai, H. 2022; 119 (15): e2123111119

  Abstract

  SignificanceSurgical removal of tumors has been performed to combat cancer for over a century by surgeons relying on visual inspection and experience to identify margins between malignant and healthy tissues. Herein, we present a rare-earth down-conversion nanoparticle-anti-CD105 conjugate for cancer targeting and a handheld imager capable of concurrent photographic imaging and fluorescence/luminescence imaging. An unprecedented tumor-to-muscle ratio was achieved by near-infrared-IIb (NIR-IIb, 1,500 to 1,700 nm) imaging during surgery, 100 times higher than previous organic dyes for unambiguous determination of tumor margin. The sensitivity/biocompatibility/safety of the probes and instrumentation developed here open a paradigm of imaging-guided surgery at the single-cell level, meeting all major requirements for clinical translation to combat cancer and save human lives.

  View details for DOI 10.1073/pnas.2123111119

  View details for PubMedID 35380898

• Exploring the performance of carbonate and ether-based electrolytes for anode-free lithium metal batteries operating under various conditions JOURNAL OF POWER SOURCES Hagos, T., Bezabh, H., Redda, H., Moges, E., Huang, W., Huang, C., Su, W., Dai, H., Hwang, B. 2021; 512

  View details for DOI 10.1016/j.jpowsour.2021.230388

  View details for Web of Science ID 000700072600006

• Highly Reversible Zn Metal Anode Stabilized by Dense and Anion-Derived Passivation Layer Obtained from Concentrated Hybrid Aqueous Electrolyte ADVANCED FUNCTIONAL MATERIALS Olbasa, B., Huang, C., Fenta, F., Jiang, S., Chala, S., Tao, H., Nikodimos, Y., Wang, C., Sheu, H., Yang, Y., Ma, T., Wu, S., Su, W., Dai, H., Hwang, B. 2021

  View details for DOI 10.1002/adfm.202103959

  View details for Web of Science ID 000712101000001

• Tuning Dynamically Formed Active Phases and Catalytic Mechanisms of In Situ Electrochemically Activated Layered Double Hydroxide for Oxygen Evolution Reaction. ACS nano Chala, S. A., Tsai, M., Olbasa, B. W., Lakshmanan, K., Huang, W., Su, W., Liao, Y., Lee, J., Dai, H., Hwang, B. J. 2021

  Abstract

  The active phase and catalytic mechanisms of Ni-based layered double hydroxide (LDH) materials for oxygen evolution reaction (OER) have no common consensus and remain controversial. Moreover, engineering the site activity and the number of active sites of LDHs is an efficient approach to advance the OER activity, as the thickness and stacking structure of the LDHs layer limit the catalytic activity. This work presents an interesting in situ approach of tuning the site activity and number of active sites of NiMn-LDHs, which exhibit the superior OER performance (onset overpotential of 0.17 V and overpotential of 0.24 V at 10 mA cm-2). The fundamental mechanistic insights and active phases during the OER process are characterized by in operando techniques along with the computational density functional theory calculations, revealing that the Ni site constitutes the OER activity and the dynamically generated NiOOH moiety is the active phase. We also prove that Ni sites undergo a reversible oxidation state under the working conditions to create active NiOOH species which catalyze the water to generate oxygen. These findings suggest that the Ni(III) phase in NiMn-LDHs is the OER active site and Mn promotes the electronic properties of Ni sites. Utilizing in situ/in operando techniques and theoretical calculation, we find that the in situ intercalation of guest anions allows the expansion of the LDH layers and keeps the active NiOOH species under the oxidation state of +3 via electron coupling, which ultimately tunes the site populations and site activity toward the superior OER activity, respectively. This work thus targets to provide insight into strategies to design the next generation of highly active catalysts for water electrolysis and fuel cell technologies.

  View details for DOI 10.1021/acsnano.1c05250

  View details for PubMedID 34515484

• Sub-10-nm graphene nanoribbons with atomically smooth edges from squashed carbon nanotubes NATURE ELECTRONICS Chen, C., Lin, Y., Zhou, W., Gong, M., He, Z., Shi, F., Li, X., Wu, J., Lam, K., Wang, J., Yang, F., Zeng, Q., Guo, J., Gao, W., Zuo, J., Liu, J., Hong, G., Antaris, A. L., Lin, M., Mao, W. L., Dai, H. 2021

  View details for DOI 10.1038/s41928-021-00633-6

  View details for Web of Science ID 000692947500001

• Rechargeable Na/Cl2 and Li/Cl2 batteries. Nature Zhu, G., Tian, X., Tai, H., Li, Y., Li, J., Sun, H., Liang, P., Angell, M., Huang, C., Ku, C., Hung, W., Jiang, S., Meng, Y., Chen, H., Lin, M., Hwang, B., Dai, H. 2021; 596 (7873): 525-530

  Abstract

  Lithium-ion batteries (LIBs) are widely used in applications ranging from electric vehicles to wearable devices. Before the invention of secondary LIBs, the primary lithium-thionyl chloride (Li-SOCl2) battery was developed in the 1970s using SOCl2 as the catholyte, lithium metal as the anode and amorphous carbon as the cathode1-7. This battery discharges by lithium oxidation and catholyte reduction to sulfur, sulfur dioxide and lithium chloride, is well known for its high energy density and is widely used in real-world applications; however, it has not been made rechargeable since its invention8-13. Here we show that with a highly microporous carbon positive electrode, a starting electrolyte composed of aluminium chloride in SOCl2 with fluoride-based additives, and either sodium or lithium as the negative electrode, we can produce a rechargeable Na/Cl2 or Li/Cl2 battery operating via redox between mainly Cl2/Cl- in the micropores of carbon and Na/Na+ or Li/Li+ redox on the sodium or lithium metal. The reversible Cl2/NaCl or Cl2/LiCl redox in the microporous carbon affords rechargeability at the positive electrodeside and the thin alkali-fluoride-doped alkali-chloride solid electrolyte interfacestabilizesthe negative electrode, both are critical to secondary alkali-metal/Cl2 batteries.

  View details for DOI 10.1038/s41586-021-03757-z

  View details for PubMedID 34433941

• Origin of shuttle-free sulfurized polyacrylonitrile in lithium-sulfur batteries (vol 492, 229508, 2021) JOURNAL OF POWER SOURCES Huang, C., Cheng, J., Su, W., Partovi-Azar, P., Kuo, L., Tsai, M., Lin, M., Jand, S., Chan, T., Wu, N., Kaghazchi, P., Dai, H., Bieker, P., Hwang, B. 2021; 495

  View details for DOI 10.1016/j.jpowsour.2021.229818

  View details for Web of Science ID 000640459700002

• Origin of shuttle-free sulfurized polyacrylonitrile in lithium-sulfur batteries JOURNAL OF POWER SOURCES Huang, C., Cheng, J., Su, W., Partovi-Azar, P., Kuo, L., Tsai, M., Lin, M., Jand, S., Chan, T., Wu, N., Kaghazchi, P., Dai, H., Bieker, P., Hwang, B. 2021; 492

  View details for DOI 10.1016/j.jpowsour.2021.229508

  View details for Web of Science ID 000635068900002

• Carbon Nanotubes-Potent Carriers for Targeted Drug Delivery in Rheumatoid Arthritis. Pharmaceutics Kofoed Andersen, C., Khatri, S., Hansen, J., Slott, S., Pavan Parvathaneni, R., Mendes, A. C., Chronakis, I. S., Hung, S., Rajasekaran, N., Ma, Z., Zhu, S., Dai, H., Mellins, E. D., Astakhova, K. 2021; 13 (4)

  Abstract

  Two types of single-walled carbon nanotubes (SWCNTs), HiPco- and carboxyl-SWCNT, are evaluated as drug carriers for the traditional anti-inflammatory drug methotrexate (MTX) and a small interfering RNA (siRNA) targeting NOTCH1 gene. The nanotubes are solubilized by PEGylation and covalently loaded with MTX. The coupling efficiency (CE%) of MTX is 77-79% for HiPco-SWCNT and 71-83% for carboxyl-SWCNT. siRNA is noncovalently attached to the nanotubes with efficiency of 90-97% for HiPco-SWCNT and 87-98% for carboxyl-SWCNT. Through whole body imaging in the second near-infrared window (NIR-II window, 1000-1700 nm), SWCNTs were found to be selectively accumulated in inflamed joints in a serum transfer mouse model. We further investigated the interactions of the siRNA/MTX loaded nanotubes with human blood and mice bone marrow cells. In human blood, both types of unloaded SWCNTs were associated with B cells, monocytes and neutrophils. Interestingly, loading with MTX suppressed SWCNTs targeting specificity to immune cells, especially B cells; in contrast, loading siRNA alone enhanced the targeting specificity. Loading both MTX and siRNA to carboxyl-SWCNT enhanced targeting specificity to neutrophils and monocytes but not B cells. The targeting specificity of SWCNTs can potentially be adjusted by altering the ratio of MTX and siRNA loaded. The combined results show that carbon nanotubes have the potential for delivery of cargo drugs specifically to immune cells involved in rheumatoid arthritis.

  View details for DOI 10.3390/pharmaceutics13040453

  View details for PubMedID 33801590

• Rational Design of High Brightness NIR-II Organic Dyes with S-D-A-D-S Structure ACCOUNTS OF MATERIALS RESEARCH Yang, Q., Ma, H., Liang, Y., Dai, H. 2021; 2 (3): 170-183

  View details for DOI 10.1021/accountsmr.0c00114

  View details for Web of Science ID 000651110500006

• Selective and High Current CO2 Electro-Reduction to Multicarbon Products in Near-Neutral KCl Electrolytes. Journal of the American Chemical Society Zhang, X., Li, J., Li, Y., Jung, Y., Kuang, Y., Zhu, G., Liang, Y., Dai, H. 2021

  Abstract

  Reducing CO2 to value-added multicarbon (C2+) fuels and chemicals using renewable energy is a viable way to circumvent CO2 buildup in the atmosphere and facilitate closing the carbon cycle. To date it remains a challenge to achieve high product selectivity and long-term stability of electrocatalytic carbon dioxide reduction reaction (CO2RR) especially at practically relevant high current levels >100 mA cm-2. Here, we report a simple electrodeposited Cu electrocatalyst on a hydrophobic porous gas-diffusion layer (GDL) electrode affording stable and selective CO2RR to C2+ products in near-neutral KCl electrolytes. By directing the CO2 stream to fully submerged hydrophobic GDLs in a H-cell, high C2+ partial current densities near 100 mA cm-2 were achieved. In a flow-cell setup, the Cu/GDL cathode in 2 M KCl afforded stable CO2RR superior to that in widely used KOH electrolytes. We found that Cu etching/corrosion associated with trace oxygen played a role in the catalyst instability in alkaline media under cathodic CO2RR conditions, a problem largely suppressed in near-neutral electrolyte. A two-electrode CO2 electrolyzer was constructed with a Cu/GDL cathode in KCl catholyte and an anode comprised of nickel-iron hydroxide on nickel foam (NiFe/NF) in a KOH anolyte separated by Nafion membrane. By periodically adding HCl to the KCl catholyte to compensate the increasing pH and remove accumulated (bi)carbonates, we observed little decay over 30 h in flow-cell CO2RR activity and selectivity at 150 mA cm-2 with a high Faradaic efficiency (FE) of 75% and energy efficiency of 40% for C2+ products.

  View details for DOI 10.1021/jacs.0c13427

  View details for PubMedID 33617245

• In vivo NIR-II structured-illumination light-sheet microscopy. Proceedings of the National Academy of Sciences of the United States of America Wang, F., Ma, Z., Zhong, Y., Salazar, F., Xu, C., Ren, F., Qu, L., Wu, A. M., Dai, H. 2021; 118 (6)

  Abstract

  Noninvasive optical imaging with deep tissue penetration depth and high spatiotemporal resolution is important to longitudinally studying the biology at the single-cell level in live mammals, but has been challenging due to light scattering. Here, we developed near-infrared II (NIR-II) (1,000 to 1,700 nm) structured-illumination light-sheet microscopy (NIR-II SIM) with ultralong excitation and emission wavelengths up to 1,540 and 1,700 nm, respectively, suppressing light scattering to afford large volumetric three-dimensional (3D) imaging of tissues with deep-axial penetration depths. Integrating structured illumination into NIR-II light-sheet microscopy further diminished background and improved spatial resolution by approximately twofold. In vivo oblique NIR-II SIM was performed noninvasively for 3D volumetric multiplexed molecular imaging of the CT26 tumor microenvironment in mice, longitudinally mapping out CD4, CD8, and OX40 at the single-cell level in response to immunotherapy by cytosine-phosphate-guanine (CpG), a Toll-like receptor 9 (TLR-9) agonist combined with OX40 antibody treatment. NIR-II SIM affords an additional tool for noninvasive volumetric molecular imaging of immune cells in live mammals.

  View details for DOI 10.1073/pnas.2023888118

  View details for PubMedID 33526701

• Deep learning for in vivo near-infrared imaging. Proceedings of the National Academy of Sciences of the United States of America Ma, Z., Wang, F., Wang, W., Zhong, Y., Dai, H. 2021; 118 (1)

  Abstract

  Detecting fluorescence in the second near-infrared window (NIR-II) up to 1,700 nm has emerged as a novel in vivo imaging modality with high spatial and temporal resolution through millimeter tissue depths. Imaging in the NIR-IIb window (1,500-1,700 nm) is the most effective one-photon approach to suppressing light scattering and maximizing imaging penetration depth, but relies on nanoparticle probes such as PbS/CdS containing toxic elements. On the other hand, imaging the NIR-I (700-1,000 nm) or NIR-IIa window (1,000-1,300 nm) can be done using biocompatible small-molecule fluorescent probes including US Food and Drug Administration-approved dyes such as indocyanine green (ICG), but has a caveat of suboptimal imaging quality due to light scattering. It is highly desired to achieve the performance of NIR-IIb imaging using molecular probes approved for human use. Here, we trained artificial neural networks to transform a fluorescence image in the shorter-wavelength NIR window of 900-1,300 nm (NIR-I/IIa) to an image resembling an NIR-IIb image. With deep-learning translation, in vivo lymph node imaging with ICG achieved an unprecedented signal-to-background ratio of >100. Using preclinical fluorophores such as IRDye-800, translation of 900-nm NIR molecular imaging of PD-L1 or EGFR greatly enhanced tumor-to-normal tissue ratio up to 20 from 5 and improved tumor margin localization. Further, deep learning greatly improved in vivo noninvasive NIR-II light-sheet microscopy (LSM) in resolution and signal/background. NIR imaging equipped with deep learning could facilitate basic biomedical research and empower clinical diagnostics and imaging-guided surgery in the clinic.

  View details for DOI 10.1073/pnas.2021446118

  View details for PubMedID 33372162

• Large-Scale Inhomogeneous Fluorescence Plasmonic Silver Chips: Origin and Mechanism CHEM Hsu, L., Yen, H., Lee, M., Sheu, Y., Chen, P., Dai, H., Chen, C. 2020; 6 (12): 3396–3408

  View details for DOI 10.1016/j.chempr.2020.10.014

  View details for Web of Science ID 000596158700018

• Resolving the Phase Instability of a Fluorinated Ether, Carbonate-Based Electrolyte for the Safe Operation of an Anode-Free Lithium Metal Battery ACS APPLIED ENERGY MATERIALS Hagos, T., Hagos, T., Bezabh, H., Berhe, G., Abrha, L., Chiu, S., Huang, C., Su, W., Dai, H., Hwang, B. 2020; 3 (11): 10722–33

  View details for DOI 10.1021/acsaem.0c01767

  View details for Web of Science ID 000595488500048

• Cross-Link-Functionalized Nanoparticles for Rapid Excretion in Nanotheranostic Applications. Angewandte Chemie (Weinheim an der Bergstrasse, Germany) Ma, Z., Wang, F., Zhong, Y., Salazar, F., Li, J., Zhang, M., Ren, F., Wu, A. M., Dai, H. 2020; 132 (46): 20733-20741

  Abstract

  Most NIR-IIb fluorophores are nanoparticle-based probes with long retention ( 1 month or longer) in the body. Here, we applied a novel cross-linked coating to functionalize core/shell lead sulfide/cadmium sulfide quantum dots (PbS/CdS QDs) emitting at 1600 nm. The coating was comprised of an amphiphilic polymer followed by three crosslinked amphiphilic polymeric layers (P3 coating), imparting high biocompatibility and > 90% excretion of QDs within 2 weeks of intravenous administration. The P3-QDs were conjugated to an engineered anti-CD8 diabody (Cys-diabody) for in vivo molecular imaging of CD8 + cytotoxic T lymphocytes (CTLs) in response to anti-PD-L1 therapy. Two-plex molecular imaging in combination with down-conversion Er nanoparticles (ErNPs) was performed for real-time in vivo monitoring of PD-L1 positive tumor cells and CTLs with cellular resolution by non-invasive NIR-IIb light sheet microscopy. Imaging of angiogenesis in the tumor microenvironment and of lymph nodes deep in the body with a signal-to-background ratio of up to 170 was also achieved using P3-QDs.

  View details for DOI 10.1002/ange.202008083

  View details for PubMedID 34334834

• A high-performance potassium metal battery using safe ionic liquid electrolyte. Proceedings of the National Academy of Sciences of the United States of America Sun, H., Liang, P., Zhu, G., Hung, W. H., Li, Y., Tai, H., Huang, C., Li, J., Meng, Y., Angell, M., Wang, C., Dai, H. 2020

  Abstract

  Potassium secondary batteries are contenders of next-generation energy storage devices owing to the much higher abundance of potassium than lithium. However, safety issues and poor cycle life of K metal battery have been key bottlenecks. Here we report an ionic liquid electrolyte comprising 1-ethyl-3-methylimidazolium chloride/AlCl3/KCl/potassium bis(fluorosulfonyl) imide for safe and high-performance batteries. The electrolyte is nonflammable and exhibits a high ionic conductivity of 13.1 mS cm-1 at room temperature. A 3.6-V battery with K anode and Prussian blue/reduced graphene oxide cathode delivers a high energy and power density of 381 and 1,350 W kg-1, respectively. The battery shows an excellent cycling stability over 820 cycles, retaining 89% of the original capacity with high Coulombic efficiencies of 99.9%. High cyclability is also achieved at elevated temperatures up to 60 °C. Uniquely, robust K, Al, F, and Cl-containing passivating interphases are afforded with this electrolyte, which is key to superior battery cycling performances.

  View details for DOI 10.1073/pnas.2012716117

  View details for PubMedID 33106405

• Electrochemical transformation reaction of Cu-MnO in aqueous rechargeable zinc-ion batteries for high performance and long cycle life JOURNAL OF MATERIALS CHEMISTRY A Fenta, F., Olbasa, B., Tsai, M., Weret, M., Zegeye, T., Huang, C., Huang, W., Zeleke, T., Sahalie, N., Pao, C., Wu, S., Su, W., Dai, H., Hwang, B. 2020; 8 (34): 17595–607

  View details for DOI 10.1039/d0ta04175k

  View details for Web of Science ID 000566092600023

• Molecular engineering of dispersed nickel phthalocyanines on carbon nanotubes for selective CO(2)reduction NATURE ENERGY Zhang, X., Wang, Y., Gu, M., Wang, M., Zhang, Z., Pan, W., Jiang, Z., Zheng, H., Lucero, M., Wang, H., Sterbinsky, G. E., Ma, Q., Wang, Y., Feng, Z., Li, J., Dai, H., Liang, Y. 2020

  View details for DOI 10.1038/s41560-020-0667-9

  View details for Web of Science ID 000558156800001

• Advancing nanomedicine with cross-link functionalized nanoparticles for rapid excretion. Angewandte Chemie (International ed. in English) Dai, H., Ma, Z., Wang, F., Zhong, Y., Salazar, F., Li, J., Zhang, M., Ren, F., Wu, A. M. 2020

  Abstract

  Nanoparticles have been widely investigated for preclinical animal models as imaging, therapeutic or theranostic agent. However, a very limited number of nanoscale materials are approved for human use due to retention and toxicity concerns. Recent years have seen in vivo fluorescence imaging in the long end of the second near infrared window (NIR-IIb, 1,500-1,700 nm), affording deeper tissue penetration and higher imaging clarity owing to reduced light scattering and near-zero autofluorescence. Most NIR-IIb fluorophores are nanoparticle based probes with long retentionin the body. Here, we applied a novel cross-linked coating to functionalize core/shell lead sulfide/cadmium sulfide quantum dots (PbS/CdS QDs) emitting at ~1,600 nm. The coating was comprised of an amphiphilic polymer followed by three crosslinked amphiphilic polymeric layers (branched PEG-linear PAA-branched PEG, P 3 coating), imparting high biocompatibility and > 90% excretion of QDs within 2 weeks of intravenous administration. The P 3 -QDs were utilized for conjugation to an engineered anti-CD8 diabody to afford in vivo molecular imaging of CD8+ cytotoxic T lymphocytes (CTLs) in response to anti-PD-L1 therapy. Two-plex molecular imaging in combination with down-conversion Er nanoparticles was performed for real-time in vivo monitoring of PD-L1+tumor cells and CD8+CTLswith cellular resolution by non-invasive NIR-IIb light sheet microscopy (LSM). In another application, angiogenesis in the tumor microenvironment was imaged with P 3 -QDs conjugated to TRC105, a chimeric monoclonal antibody against CD105. Further, P 3 -QDs afforded imaging of lymph nodes deep in the body with a signal-to-background ratio of up to ~170. Lastly, we show that the P 3 coating on magnetic nanoparticles also afforded rapid excretion in < 2 weeks, establishing generality of the approach. The ability of eliminating various nanoparticles from a body opens up many possibilities of nanomedicine for human use.

  View details for DOI 10.1002/anie.202008083

  View details for PubMedID 32681553

• High-Rate and Long-Cycle Stability with a Dendrite-Free Zinc Anode in an Aqueous Zn-Ion Battery Using Concentrated Electrolytes ACS APPLIED ENERGY MATERIALS Olbasa, B., Fenta, F., Chiu, S., Tsai, M., Huang, C., Jote, B., Beyene, T., Liao, Y., Wang, C., Su, W., Dai, H., Hwang, B. 2020; 3 (5): 4499–4508

  View details for DOI 10.1021/acsaem.0c00183

  View details for Web of Science ID 000537656400051

• High-Safety and High-Energy-Density Lithium Metal Batteries in a Novel Ionic-Liquid Electrolyte. Advanced materials (Deerfield Beach, Fla.) Sun, H., Zhu, G., Zhu, Y., Lin, M., Chen, H., Li, Y., Hung, W. H., Zhou, B., Wang, X., Bai, Y., Gu, M., Huang, C., Tai, H., Xu, X., Angell, M., Shyue, J., Dai, H. 2020: e2001741

  Abstract

  Rechargeable lithium metal batteries are next generation energy storage devices with high energy density, but face challenges in achieving high energy density, high safety, and long cycle life. Here, lithium metal batteries in a novel nonflammable ionic-liquid (IL) electrolyte composed of 1-ethyl-3-methylimidazolium (EMIm) cations and high-concentration bis(fluorosulfonyl)imide (FSI) anions, with sodium bis(trifluoromethanesulfonyl)imide (NaTFSI) as a key additive are reported. The Na ion participates in the formation of hybrid passivation interphases and contributes to dendrite-free Li deposition and reversible cathode electrochemistry. The electrolyte of low viscosity allows practically useful cathode mass loading up to 16 mg cm-2 . Li anodes paired with lithium cobalt oxide (LiCoO2 ) and lithium nickel cobalt manganese oxide (LiNi0.8 Co0.1 Mn0.1 O2 , NCM 811) cathodes exhibit 99.6-99.9% Coulombic efficiencies, high discharge voltages up to 4.4 V, high specific capacity and energy density up to 199 mAh g-1 and 765 Wh kg-1 respectively, with impressive cycling performances over up to 1200 cycles. Highly stable passivation interphases formed on both electrodes in the novel IL electrolyte are the key to highly reversible lithium metal batteries, especially for Li-NMC 811 full batteries.

  View details for DOI 10.1002/adma.202001741

  View details for PubMedID 32449260

• A mini-review on rare-earth down-conversion nanoparticles for NIR-II imaging of biological systems. Nano research Zhong, Y., Dai, H. 2020; 13 (5): 1281-1294

  Abstract

  Rare-earth (RE) based luminescent probes exhibit rich optical properties including upconversion and down-conversion luminescence spanning a broad spectral range from 300 to 3,000 nm, and have generated great scientific and practical interest from telecommunication to biological imaging. While upconversion nanoparticles have been investigated for decades, down-conversion luminescence of RE-based probes in the second near-infrared (NIR-II, 1,000-1,700 nm) window for in vivo biological imaging with sub-centimeter tissue penetration and micrometer image resolution has come into light only recently. In this review, we present recent progress on RE-based NIR-II probes for in vivo vasculature and molecular imaging with a focus on Er3+-based nanoparticles due to the down-conversion luminescence at the long-wavelength end of the NIR-II window (NIR-IIb, 1,500-1,700 nm). Imaging in NIR-IIb is superior to imaging with organic probes such as ICG and IRDye800 in the ~ 800 nm NIR range and the 1,000-1,300 nm short end of NIR-II range, owing to minimized light scattering and autofluorescence background. Doping by cerium and other ions and phase engineering of Er3+-based nanoparticles, combined with surface hydrophilic coating optimization can afford ultrabright, biocompatible NIR-IIb probe towards clinical translation for human use. The Nd3+-based probes with NIR-II emission at 1,050 and 1,330 nm are also discussed, including Nd3+ doped nanocrystals and Nd3+-organic ligand complexes. This review also points out future directions for further development of multi-functional RE NIR-II probes for biological imaging.

  View details for DOI 10.1007/s12274-020-2721-0

  View details for PubMedID 34336144

  View details for PubMedCentralID PMC8323785

• A mini-review on rare-earth down-conversion nanoparticles for NIR-II imaging of biological systems NANO RESEARCH Zhong, Y., Dai, H. 2020

  View details for DOI 10.1007/s12274-020-2721-0

  View details for Web of Science ID 000525341500001

• Carbon-coated FeCo nanoparticles as sensitive magnetic-particle-imaging tracers with photothermal and magnetothermal properties. Nature biomedical engineering Song, G. n., Kenney, M. n., Chen, Y. S., Zheng, X. n., Deng, Y. n., Chen, Z. n., Wang, S. X., Gambhir, S. S., Dai, H. n., Rao, J. n. 2020

  Abstract

  The low magnetic saturation of iron oxide nanoparticles, which are developed primarily as contrast agents for magnetic resonance imaging, limits the sensitivity of their detection using magnetic particle imaging (MPI). Here, we show that FeCo nanoparticles that have a core diameter of 10 nm and bear a graphitic carbon shell decorated with poly(ethylene glycol) provide an MPI signal intensity that is sixfold and fifteenfold higher than the signals from the superparamagnetic iron oxide tracers VivoTrax and Feraheme, respectively, at the same molar concentration of iron. We also show that the nanoparticles have photothermal and magnetothermal properties and can therefore be used for tumour ablation in mice, and that they have high optical absorbance in a broad near-infrared region spectral range (wavelength, 700-1,200 nm), making them suitable as tracers for photoacoustic imaging. As sensitive multifunctional and multimodal imaging tracers, carbon-coated FeCo nanoparticles may confer advantages in cancer imaging and hyperthermia therapy.

  View details for DOI 10.1038/s41551-019-0506-0

  View details for PubMedID 32015409

• Hierarchical 3D Architectured Ag Nanowires Shelled with NiMn-Layered Double Hydroxide as an Efficient Bifunctional Oxygen Electrocatalyst. ACS nano Chala, S. A., Tsai, M. C., Su, W. N., Ibrahim, K. B., Thirumalraj, B. n., Chan, T. S., Lee, J. F., Dai, H. n., Hwang, B. J. 2020

  Abstract

  Herein, we report hierarchical 3D NiMn-layered double hydroxide (NiMn-LDHs) shells grown on conductive silver nanowire (Ag NWs) cores as efficient, low-cost, and durable oxygen reduction reaction (ORR)/oxygen evolution reaction (OER) bifunctional electrocatalysts for metal-air batteries. The hierarchical 3D architectured Ag NW@NiMn-LDH catalysts exhibit superb OER/ORR activities in alkaline conditions. The outstanding bifunctional activities of Ag NW@NiMn-LDHs are essentially attributed to increasing both site activity and site populations. The synergistic contributions from the hierarchical 3D open-pore structure of the LDH shells, improved electrical conductivity, and small thickness of the LDHs shells are associated with more accessible site populations. Moreover, the charge transfer between Ag cores and metals of LDH shells and the formation of defective and distorted sites (less coordinated Ni and Mn sites) strongly enhance the site activity. Thus, Ag NW@NiMn-LDH hybrids exhibit a 0.75 V overvoltage difference between ORR and OER with excellent durability for 30 h, demonstrating the distinguished bifunctional electrocatalyst reported to date. Interestingly, the homemade rechargeable Zn-air battery using the hybrid Ag NW@NiMn-LDHs (1:2) catalyst as the air electrode exhibits a charge-discharge voltage gap of ∼0.77 V at 10 mA cm-2 and shows excellent cycling stability. Thus, the concept of the hierarchical 3D architecture of Ag NW@NiMn-LDHs considerably advances the practice of LDHs toward metal-air batteries and oxygen electrocatalysts.

  View details for DOI 10.1021/acsnano.9b07487

  View details for PubMedID 32003975

• Electroreduction of CO2 to Formate on a Copper-Based Electrocatalyst at High Pressures with High Energy Conversion Efficiency. Journal of the American Chemical Society Li, J. n., Kuang, Y. n., Meng, Y. n., Tian, X. n., Hung, W. H., Zhang, X. n., Li, A. n., Xu, M. n., Zhou, W. n., Ku, C. S., Chiang, C. Y., Zhu, G. n., Guo, J. n., Sun, X. n., Dai, H. n. 2020

  Abstract

  Electrocatalytic CO2 reduction (CO2RR) to valuable fuels is a promising approach to mitigate energy and environmental problems, but controlling the reaction pathways and products remains challenging. Here a novel Cu2O nanoparticle film was synthesized by square-wave (SW) electrochemical redox cycling of high-purity Cu foils. The cathode afforded up to 98% Faradaic efficiency for electroreduction of CO2 to nearly pure formate under ≥45 atm CO2 in bicarbonate catholytes. When this cathode was paired with a newly developed NiFe hydroxide carbonate anode in KOH/borate anolyte, the resulting two-electrode high-pressure electrolysis cell achieved high energy conversion efficiencies of up to 55.8% stably for long-term formate production. While the high-pressure conditions drastically increased the solubility of CO2 to enhance CO2 reduction and suppress hydrogen evolution, the (111)-oriented Cu2O film was found to be important to afford nearly 100% CO2 reduction to formate. The results have implications for CO2 reduction to a single liquid product with high energy conversion efficiency.

  View details for DOI 10.1021/jacs.0c00122

  View details for PubMedID 32250611

• Quantification of antibody avidities and accurate detection of SARS-CoV-2 antibodies in serum and saliva on plasmonic substrates. Nature biomedical engineering Liu, T. n., Hsiung, J. n., Zhao, S. n., Kost, J. n., Sreedhar, D. n., Hanson, C. V., Olson, K. n., Keare, D. n., Chang, S. T., Bliden, K. P., Gurbel, P. A., Tantry, U. S., Roche, J. n., Press, C. n., Boggs, J. n., Rodriguez-Soto, J. P., Montoya, J. G., Tang, M. n., Dai, H. n. 2020

  Abstract

  Accurate assays for the detection of antibodies to SARS-CoV-2 (severe acute respiratory syndrome coronavirus 2) are essential for the control of the COVID-19 (coronavirus disease 2019) pandemic. Here, we report antibody and antibody-avidity assays, relying on near-infrared-fluorescence amplification by nanostructured plasmonic gold substrates, for the simultaneous detection of antibodies to the S1 subunit of the spike protein and to the receptor binding domain of SARS-CoV-2 in human serum and saliva, and for quantifying immunoglobulin avidities against coronavirus antigens from SARS-CoV-2, SARS-CoV-1 and the common-cold viruses OC43, HKU1, NL63 and 229E. The antibody assay detected immunoglobulin M in 87% (52 of 60) COVID-19-positive serum samples collected 6 or more days after symptom onset (and the immunoglobulins M and G in all 33 samples collected at least 15 days after symptom onset), and correctly classified 456 out of the 457 COVID-19-negative serum samples tested (424 of them collected before the pandemic, including 73 that were positive for other viruses). We used the antibody-avidity assay to study antibody-maturation patterns, anamnestic responses, and cross-immunity to the common-cold coronaviruses.

  View details for DOI 10.1038/s41551-020-00642-4

  View details for PubMedID 33122853

• Diagnosis and prognosis of myocardial infarction on a plasmonic chip. Nature communications Xu, W. n., Wang, L. n., Zhang, R. n., Sun, X. n., Huang, L. n., Su, H. n., Wei, X. n., Chen, C. C., Lou, J. n., Dai, H. n., Qian, K. n. 2020; 11 (1): 1654

  Abstract

  Cardiovascular diseases lead to 31.5% of deaths globally, and particularly myocardial infarction (MI) results in 7.4 million deaths per year. Diagnosis of MI and monitoring for prognostic use are critical for clinical management and biomedical research, which require advanced tools with accuracy and speed. Herein, we developed a plasmonic gold nano-island (pGold) chip assay for diagnosis and monitoring of MI. On-chip microarray analysis of serum biomarkers (e.g., cardiac troponin I) afforded up to 130-fold enhancement of near-infrared fluorescence for ultra-sensitive and quantitative detection within controlled periods, using 10 μL of serum only. The pGold chip assay achieved MI diagnostic sensitivity of 100% and specificity of 95.54%, superior to the standard chemiluminescence immunoassay in cardiovascular clinics. Further, we monitored biomarker concentrations regarding percutaneous coronary intervention for prognostic purpose. Our work demonstrated a designed approach using plasmonic materials for enhanced diagnosis and monitoring for prognostic use towards point-of-care testing.

  View details for DOI 10.1038/s41467-020-15487-3

  View details for PubMedID 32245966

• Highly active oxygen evolution integrated with efficient CO2 to CO electroreduction. Proceedings of the National Academy of Sciences of the United States of America Meng, Y., Zhang, X., Hung, W., He, J., Tsai, Y., Kuang, Y., Kenney, M. J., Shyue, J., Liu, Y., Stone, K. H., Zheng, X., Suib, S. L., Lin, M., Liang, Y., Dai, H. 2019

  Abstract

  Electrochemical reduction of CO2 to useful chemicals has been actively pursued for closing the carbon cycle and preventing further deterioration of the environment/climate. Since CO2 reduction reaction (CO2RR) at a cathode is always paired with the oxygen evolution reaction (OER) at an anode, the overall efficiency of electrical energy to chemical fuel conversion must consider the large energy barrier and sluggish kinetics of OER, especially in widely used electrolytes, such as the pH-neutral CO2-saturated 0.5 M KHCO3 OER in such electrolytes mostly relies on noble metal (Ir- and Ru-based) electrocatalysts in the anode. Here, we discover that by anodizing a metallic Ni-Fe composite foam under a harsh condition (in a low-concentration 0.1 M KHCO3 solution at 85 °C under a high-current 250 mA/cm2), OER on the NiFe foam is accompanied by anodic etching, and the surface layer evolves into a nickel-iron hydroxide carbonate (NiFe-HC) material composed of porous, poorly crystalline flakes of flower-like NiFe layer-double hydroxide (LDH) intercalated with carbonate anions. The resulting NiFe-HC electrode in CO2-saturated 0.5 M KHCO3 exhibited OER activity superior to IrO2, with an overpotential of 450 and 590 mV to reach 10 and 250 mA/cm2, respectively, and high stability for >120 h without decay. We paired NiFe-HC with a CO2RR catalyst of cobalt phthalocyanine/carbon nanotube (CoPc/CNT) in a CO2 electrolyzer, achieving selective cathodic conversion of CO2 to CO with >97% Faradaic efficiency and simultaneous anodic water oxidation to O2 The device showed a low cell voltage of 2.13 V and high electricity-to-chemical fuel efficiency of 59% at a current density of 10 mA/cm2.

  View details for DOI 10.1073/pnas.1915319116

  View details for PubMedID 31723041

• Ionic Liquid Analogs of AlCl3 with Urea Derivatives as Electrolytes for Aluminum Batteries ADVANCED FUNCTIONAL MATERIALS Angell, M., Zhu, G., Lin, M., Rong, Y., Dai, H. 2019

  View details for DOI 10.1002/adfm.201901928

  View details for Web of Science ID 000492962900001

• In vivo molecular imaging for immunotherapy using ultra-bright near-infrared-IIb rare-earth nanoparticles. Nature biotechnology Zhong, Y., Ma, Z., Wang, F., Wang, X., Yang, Y., Liu, Y., Zhao, X., Li, J., Du, H., Zhang, M., Cui, Q., Zhu, S., Sun, Q., Wan, H., Tian, Y., Liu, Q., Wang, W., Garcia, K. C., Dai, H. 2019

  Abstract

  The near-infrared-IIb (NIR-IIb) (1,500-1,700nm) window is ideal for deep-tissue optical imaging in mammals, but lacks bright and biocompatible probes. Here, we developed biocompatible cubic-phase (alpha-phase) erbium-based rare-earth nanoparticles (ErNPs) exhibiting bright downconversion luminescence at ~1,600nm for dynamic imaging of cancer immunotherapy in mice. We used ErNPs functionalized with cross-linked hydrophilic polymer layers attached to anti-PD-L1 (programmed cell death-1 ligand-1) antibody for molecular imaging of PD-L1 in a mouse model of colon cancer and achieved tumor-to-normal tissue signal ratios of ~40. The long luminescence lifetime of ErNPs (~4.6ms) enabled simultaneous imaging of ErNPs and lead sulfide quantum dots emitting in the same ~1,600nm window. In vivo NIR-IIb molecular imaging of PD-L1 and CD8 revealed cytotoxic T lymphocytes in the tumor microenvironment in response to immunotherapy, and altered CD8 signals in tumor and spleen due to immune activation. The cross-linked functionalization layer facilitated 90% ErNP excretion within 2weeks without detectable toxicity in mice.

  View details for DOI 10.1038/s41587-019-0262-4

  View details for PubMedID 31570897

• The Nano Research Young Innovators (NR45) Awards in nanoenergy NANO RESEARCH Wang, H., Dai, H. 2019; 12 (9): 1975–77

  View details for DOI 10.1007/s12274-019-2475-8

  View details for Web of Science ID 000485041800001

• Dual electrolyte additives of potassium hexafluorophosphate and tris (trimethylsilyl) phosphite for anode-free lithium metal batteries ELECTROCHIMICA ACTA Hagos, T., Berhe, G., Hagos, T., Bezabh, H., Abrha, L., Beyene, T., Huang, C., Yang, Y., Su, W., Dai, H., Hwang, B. 2019; 316: 52–59

  View details for DOI 10.1016/j.electacta.2019.05.061

  View details for Web of Science ID 000471118900006

• A safe and non-flammable sodium metal battery based on an ionic liquid electrolyte. Nature communications Sun, H., Zhu, G., Xu, X., Liao, M., Li, Y., Angell, M., Gu, M., Zhu, Y., Hung, W. H., Li, J., Kuang, Y., Meng, Y., Lin, M., Peng, H., Dai, H. 2019; 10 (1): 3302

  Abstract

  Rechargeable sodium metal batteries with high energy density could be important to a wide range of energy applications in modern society. The pursuit of higher energy density should ideally come with high safety, a goal difficult for electrolytes based on organic solvents. Here we report a chloroaluminate ionic liquid electrolyte comprised of aluminium chloride/1-methyl-3-ethylimidazolium chloride/sodium chloride ionic liquid spiked with two important additives, ethylaluminum dichloride and 1-ethyl-3-methylimidazolium bis(fluorosulfonyl)imide. This leads to the first chloroaluminate based ionic liquid electrolyte for rechargeable sodium metal battery. The obtained batteries reached voltages up to ~4V, high Coulombic efficiency up to 99.9%, and high energy and power density of ~420Whkg-1 and ~1766 W kg-1, respectively. The batteries retained over 90% of the original capacity after 700 cycles, suggesting an effective approach to sodium metal batteries with high energy/high power density, long cycle life and high safety.

  View details for DOI 10.1038/s41467-019-11102-2

  View details for PubMedID 31341162

• Molecular imaging in the second near-infrared window. Advanced functional materials Wan, H., Du, H., Wang, F., Dai, H. 2019; 29 (25)

  Abstract

  In the past decade, noticeable progress has been achieved regarding fluorescence imaging in the second near-infrared (NIR-II) window. Fluorescence imaging in the NIR-II window demonstrates superiorities of deep tissue penetration and high spatial and temporal resolution, which are beneficial for profiling physiological processes. Meanwhile, molecular imaging has emerged as an efficient tool to decipher biological activities on the molecular and cellular level. Extending molecular imaging into the NIR-II window would enhance the imaging performance, providing more detailed and accurate information of the biological system. In this progress report, selected achievements made in NIR-II molecular imaging are summarized. The organization of this report is based on strategies underlying rational designs of NIR-II imaging probes and their applications in molecular imaging are highlighted. This progress report may provide guidance and reference for further development of functional NIR-II probes designed for high-performance molecular imaging.

  View details for DOI 10.1002/adfm.201900566

  View details for PubMedID 31885529

  View details for PubMedCentralID PMC6934177

• Molecular Imaging in the Second Near-Infrared Window ADVANCED FUNCTIONAL MATERIALS Wan, H., Du, H., Wang, F., Dai, H. 2019; 29 (25)

  View details for DOI 10.1002/adfm.201900566

  View details for Web of Science ID 000472552900017

• An electrodeposition approach to metal/metal oxide heterostructures for active hydrogen evolution catalysts in near-neutral electrolytes NANO RESEARCH Kenney, M. J., Huang, J., Zhu, Y., Meng, Y., Xu, M., Zhu, G., Hung, W., Kuang, Y., Lin, M., Sun, X., Zhou, W., Dai, H. 2019; 12 (6): 1431–35

  View details for DOI 10.1007/s12274-019-2379-7

  View details for Web of Science ID 000469405300026

• Light-sheet microscopy in the near-infrared II window NATURE METHODS Wang, F., Wan, H., Ma, Z., Zhong, Y., Sun, Q., Tian, Y., Qu, L., Du, H., Zhang, M., Li, L., Ma, H., Luo, J., Liang, Y., Li, W., Hong, G., Liu, L., Dai, H. 2019; 16 (6): 545-+

  View details for DOI 10.1038/s41592-019-0398-7

  View details for Web of Science ID 000469455200024

• Near-Infrared-II Molecular Dyes for Cancer Imaging and Surgery ADVANCED MATERIALS Zhu, S., Tian, R., Antaris, A. L., Chen, X., Dai, H. 2019; 31 (24)

  View details for DOI 10.1002/adma.201900321

  View details for Web of Science ID 000485478200011

• Light-sheet microscopy in the near-infrared II window. Nature methods Wang, F., Wan, H., Ma, Z., Zhong, Y., Sun, Q., Tian, Y., Qu, L., Du, H., Zhang, M., Li, L., Ma, H., Luo, J., Liang, Y., Li, W. J., Hong, G., Liu, L., Dai, H. 2019

  Abstract

  Non-invasive deep-tissue three-dimensional optical imaging of live mammals with high spatiotemporal resolution is challenging owing to light scattering. We developed near-infrared II (1,000-1,700nm) light-sheet microscopy with excitation and emission of up to approximately 1,320nm and 1,700nm, respectively, for optical sectioning at a penetration depth of approximately 750mum through live tissues without invasive surgery and at a depth of approximately 2mm in glycerol-cleared brain tissues. Near-infrared II light-sheet microscopy in normal and oblique configurations enabled in vivo imaging of live mice through intact tissue, revealing abnormal blood flow and T-cell motion in tumor microcirculation and mapping out programmed-death ligand 1 and programmed cell death protein 1 in tumors with cellular resolution. Three-dimensional imaging through the intact mouse head resolved vascular channels between the skull and brain cortex, and allowed monitoring of recruitment of macrophages and microglia to the traumatic brain injury site.

  View details for PubMedID 31086342

• Concentrated Dual-Salt Electrolyte to Stabilize Li Metal and Increase Cycle Life of Anode Free Li-Metal Batteries JOURNAL OF THE ELECTROCHEMICAL SOCIETY Beyene, T., Bezabh, H., Weret, M., Hagos, T., Huang, C., Wang, C., Su, W., Dai, H., Hwang, B. 2019; 166 (8): A1501–A1509

  View details for DOI 10.1149/2.0731908jes

  View details for Web of Science ID 000466837500005

• Plasmonic gold chips for the diagnosis of Toxoplasma gondii, CMV, and rubella infections using saliva with serum detection precision EUROPEAN JOURNAL OF CLINICAL MICROBIOLOGY & INFECTIOUS DISEASES Li, X., Pomares, C., Peyron, F., Press, C. J., Ramirez, R., Geraldine, G., Cannavo, I., Chapey, E., Levigne, P., Wallon, M., Montoya, J. G., Dai, H. 2019; 38 (5): 883–90

  View details for DOI 10.1007/s10096-019-03487-1

  View details for Web of Science ID 000464869000009

• Rechargeable aluminum batteries: effects of cations in ionic liquid electrolytes. RSC advances Zhu, G., Angell, M., Pan, C. J., Lin, M. C., Chen, H., Huang, C. J., Lin, J., Achazi, A. J., Kaghazchi, P., Hwang, B. J., Dai, H. 2019; 9 (20): 11322-11330

  Abstract

  Room temperature ionic liquids (RTILs) are solvent-free liquids comprised of densely packed cations and anions. The low vapor pressure and low flammability make ILs interesting for electrolytes in batteries. In this work, a new class of ionic liquids were formed for rechargeable aluminum/graphite battery electrolytes by mixing 1-methyl-1-propylpyrrolidinium chloride (Py13Cl) with various ratios of aluminum chloride (AlCl3) (AlCl3/Py13Cl molar ratio = 1.4 to 1.7). Fundamental properties of the ionic liquids, including density, viscosity, conductivity, anion concentrations and electrolyte ion percent were investigated and compared with the previously investigated 1-ethyl-3-methylimidazolium chloride (EMIC-AlCl3) ionic liquids. The results showed that the Py13Cl-AlCl3 ionic liquid exhibited lower density, higher viscosity and lower conductivity than its EMIC-AlCl3 counterpart. We devised a Raman scattering spectroscopy method probing ILs over a Si substrate, and by using the Si Raman scattering peak for normalization, we quantified speciation including AlCl4 -, Al2Cl7 -, and larger AlCl3 related species with the general formula (AlCl3) n in different IL electrolytes. We found that larger (AlCl3) n species existed only in the Py13Cl-AlCl3 system. We propose that the larger cationic size of Py13+ (142 Å3) versus EMI+ (118 Å3) dictated the differences in the chemical and physical properties of the two ionic liquids. Both ionic liquids were used as electrolytes for aluminum-graphite batteries, with the performances of batteries compared. The chloroaluminate anion-graphite charging capacity and cycling stability of the two batteries were similar. The Py13Cl-AlCl3 based battery showed a slightly larger overpotential than EMIC-AlCl3, leading to lower energy efficiency resulting from higher viscosity and lower conductivity. The results here provide fundamental insights into ionic liquid electrolyte design for optimal battery performance.

  View details for DOI 10.1039/c9ra00765b

  View details for PubMedID 35520252

  View details for PubMedCentralID PMC9062991

• Solar-driven, highly sustained splitting of seawater into hydrogen and oxygen fuels PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Kuang, Y., Kenney, M. J., Meng, Y., Hung, W., Liu, Y., Huang, J., Prasanna, R., Li, P., Li, Y., Wang, L., Lin, M., McGehee, M. D., Sun, X., Dai, H. 2019; 116 (14): 6624–29

  View details for DOI 10.1073/pnas.1900556116

  View details for Web of Science ID 000463069900024

• A general route via formamide condensation to prepare atomically dispersed metal-nitrogen-carbon electrocatalysts for energy technologies ENERGY & ENVIRONMENTAL SCIENCE Zhang, G., Jia, Y., Zhang, C., Xiong, X., Sun, K., Chen, R., Chen, W., Kuang, Y., Zheng, L., Tang, H., Liu, W., Liu, J., Sun, X., Lin, W., Dai, H. 2019; 12 (4): 1317–25

  View details for DOI 10.1039/c9ee00162j

  View details for Web of Science ID 000465275800011

• Layered double hydroxide nanosheets decorated with metal or metal oxides for oxygen evolution and reduction reactions Chala, S., Tsai, M., Su, W., Dai, H., Hwang, B. AMER CHEMICAL SOC. 2019

  View details for Web of Science ID 000478860502402

• Solar-driven, highly sustained splitting of seawater into hydrogen and oxygen fuels. Proceedings of the National Academy of Sciences of the United States of America Kuang, Y., Kenney, M. J., Meng, Y., Hung, W., Liu, Y., Huang, J. E., Prasanna, R., Li, P., Li, Y., Wang, L., Lin, M., McGehee, M. D., Sun, X., Dai, H. 2019

  Abstract

  Electrolysis of water to generate hydrogen fuel is an attractive renewable energy storage technology. However, grid-scale freshwater electrolysis would put a heavy strain on vital water resources. Developing cheap electrocatalysts and electrodes that can sustain seawater splitting without chloride corrosion could address the water scarcity issue. Here we present a multilayer anode consisting of a nickel-iron hydroxide (NiFe) electrocatalyst layer uniformly coated on a nickel sulfide (NiSx) layer formed on porous Ni foam (NiFe/NiSx-Ni), affording superior catalytic activity and corrosion resistance in solar-driven alkaline seawater electrolysis operating at industrially required current densities (0.4 to 1 A/cm2) over 1,000 h. A continuous, highly oxygen evolution reaction-active NiFe electrocatalyst layer drawing anodic currents toward water oxidation and an in situ-generated polyatomic sulfate and carbonate-rich passivating layers formed in the anode are responsible for chloride repelling and superior corrosion resistance of the salty-water-splitting anode.

  View details for PubMedID 30886092

• Stabilizing Lithium into Cross-Stacked Nanotube Sheets with an Ultra-High Specific Capacity for Lithium Oxygen Batteries ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Ye, L., Liao, M., Sun, H., Yang, Y., Tang, C., Zhao, Y., Wang, L., Xu, Y., Zhang, L., Wang, B., Xu, F., Sun, X., Zhang, Y., Dai, H., Bruce, P. G., Peng, H. 2019; 58 (8): 2437–42

  View details for DOI 10.1002/anie.201814324

  View details for Web of Science ID 000458417700045

• Magnetic "Squashing" of Circulating Tumor Cells on Plasmonic Substrates for Ultrasensitive NIR Fluorescence Detection SMALL METHODS Zhang, R., Le, B., Xu, W., Guo, K., Sun, X., Su, H., Huang, L., Huang, J., Shen, T., Liao, T., Liang, Y., Zhang, J. J., Dai, H., Qian, K. 2019; 3 (2)

  View details for DOI 10.1002/smtd.201800474

  View details for Web of Science ID 000458557500011

• A theranostic agent for cancer therapy and imaging in the second near-infrared window. Nano research Ma, Z., Wan, H., Wang, W., Zhang, X., Uno, T., Yang, Q., Yue, J., Gao, H., Zhong, Y., Tian, Y., Sun, Q., Liang, Y., Dai, H. 2019; 12: 273-279

  Abstract

  Theranostic nanoparticles are integrated systems useful for simultaneous diagnosis and imaging guided delivery of therapeutic drugs, with wide ranging potential applications in the clinic. Here we developed a theranostic nanoparticle (~ 24 nm size by dynamic light scattering) p-FE-PTX-FA based on polymeric micelle encapsulating an organic dye (FE) fluorescing in the 1,000-1,700 nm second near-infrared (NIR-II) window and an anti-cancer drug paclitaxel. Folic acid (FA) was conjugated to the nanoparticles to afford specific binding to molecular folate receptors on murine breast cancer 4T1 tumor cells. In vivo, the nanoparticles accumulated in 4T1 tumor through both passive and active targeting effect. Under an 808 nm laser excitation, fluorescence detection above 1,300 nm afforded a large Stokes shift, allowing targeted molecular imaging tumor with high signal to background ratios, reaching a high tumor to normal tissue signal ratio (T/NT) of (20.0 ± 2.3). Further, 4T1 tumors on mice were completed eradicated by paclitaxel released from p-FE-PTA-FA within 20 days of the first injection. Pharmacokinetics and histology studies indicated p-FE-PTX-FA had no obvious toxic side effects to major organs. This represented the first NIR-II theranostic agent developed.

  View details for DOI 10.1007/s12274-018-2210-x

  View details for PubMedID 31832124

  View details for PubMedCentralID PMC6907162

• A theranostic agent for cancer therapy and imaging in the second near-infrared window NANO RESEARCH Ma, Z., Wan, H., Wang, W., Zhang, X., Uno, T., Yang, Q., Yue, J., Gao, H., Zhong, Y., Tian, Y., Sun, Q., Liang, Y., Dai, H. 2019; 12 (2): 273–79

  View details for DOI 10.1007/s12274-018-2210-x

  View details for Web of Science ID 000455549200004

• Plasmonic gold chips for the diagnosis of Toxoplasma gondii, CMV, and rubella infections using saliva with serum detection precision. European journal of clinical microbiology & infectious diseases : official publication of the European Society of Clinical Microbiology Li, X., Pomares, C., Peyron, F., Press, C. J., Ramirez, R., Geraldine, G., Cannavo, I., Chapey, E., Levigne, P., Wallon, M., Montoya, J. G., Dai, H. 2019

  Abstract

  Sampling the blood compartment by an invasive procedure such as phlebotomy is the most common approach used for diagnostic purposes. However, phlebotomy has several drawbacks including pain, vasovagal reactions, and anxiety. Therefore, alternative approaches should be tested to minimize patient's discomfort. Saliva is a reasonable compartment; when obtained, it generates little or no anxiety. We setup a multiplexed serology assay for detection of Toxoplasma gondii IgG and IgM, rubella IgG, and CMV IgG, in serum, whole blood, and saliva using novel plasmonic gold (pGOLD) chips. pGOLD test results in serum, whole blood, and saliva were compared with commercial kits test results in serum. One hundred twenty serum/saliva sets (Lyon) and 28 serum/whole blood/saliva sets (Nice) from France were tested. In serum and whole blood, sensitivity and specificity of multiplex T. gondii, CMV, and rubella IgG were 100% in pGOLD when compared to commercial test results in serum. In saliva, sensitivity and specificity for T. gondii and rubella IgG were 100%, and for CMV IgG, sensitivity and specificity were 92.9% and 100%, respectively, when compared to commercial test results in serum. We were also able to detect T. gondii IgM in saliva with sensitivity and specificity of 100% and 95.4%, respectively, when compared to serum test results. Serological testing by multiplex pGOLD assay for T. gondii, rubella, and CMV in saliva is reliable and likely to be more acceptable for systematic screening of pregnant women, newborn, and immunocompromised patients.

  View details for PubMedID 30701339

• Near-Infrared-II Molecular Dyes for Cancer Imaging and Surgery. Advanced materials (Deerfield Beach, Fla.) Zhu, S. n., Tian, R. n., Antaris, A. L., Chen, X. n., Dai, H. n. 2019: e1900321

  Abstract

  Fluorescence bioimaging affords a vital tool for both researchers and surgeons to molecularly target a variety of biological tissues and processes. This review focuses on summarizing organic dyes emitting at a biological transparency window termed the near-infrared-II (NIR-II) window, where minimal light interaction with the surrounding tissues allows photons to travel nearly unperturbed throughout the body. NIR-II fluorescence imaging overcomes the penetration/contrast bottleneck of imaging in the visible region, making it a remarkable modality for early diagnosis of cancer and highly sensitive tumor surgery. Due to their convenient bioconjugation with peptides/antibodies, NIR-II molecular dyes are desirable candidates for targeted cancer imaging, significantly overcoming the autofluorescence/scattering issues for deep tissue molecular imaging. To promote the clinical translation of NIR-II bioimaging, advancements in the high-performance small molecule-derived probes are critically important. Here, molecules with clinical potential for NIR-II imaging are discussed, summarizing the synthesis and chemical structures of NIR-II dyes, chemical and optical properties of NIR-II dyes, bioconjugation and biological behavior of NIR-II dyes, whole body imaging with NIR-II dyes for cancer detection and surgery, as well as NIR-II fluorescence microscopy imaging. A key perspective on the direction of NIR-II molecular dyes for cancer imaging and surgery is also discussed.

  View details for PubMedID 31025403

• Effects of Concentrated Salt and Resting Protocol on Solid Electrolyte Interface Formation for Improved Cycle Stability of Anode-Free Lithium Metal Batteries. ACS applied materials & interfaces Beyene, T. T., Jote, B. A., Wondimkun, Z. T., Olbassa, B. W., Huang, C. J., Thirumalraj, B. n., Wang, C. H., Su, W. N., Dai, H. n., Hwang, B. J. 2019

  Abstract

  The combined effect of concentrated electrolyte and cycling protocol on the cyclic performance of the anode-free battery (AFB) is evaluated systematically. In situ deposition of Li in the AFB configuration in the presence of a concentrated electrolyte containing fluorine-donating salt and resting the deposit enables the formation of stable and uniform SEI. The SEI intercepts the undesirable side reaction between the deposit and solvent in the electrolyte and reduces electrolyte and Li consumption during cycling. The synergy between the laboratory-prepared concentrated 3 M LiFSI in the ester-based electrolyte and our resting protocol significantly enhanced cyclic performances of AFBs in comparison to the commercial carbonate-based dilute electrolyte, 1 M LiPF6. Benefitting from the combined effect, Cu∥LiFePO4 cells delivered excellent cyclic performance at 0.5 mA/cm2 with an average CE of up to 98.78%, retaining a reasonable discharge capacity after 100 cycles. Furthermore, the AFB can also be cycled at a high rate up to 1.0 mA/cm2 with a high average CE and retaining the encouraging discharge capacity after 100 cycles. The fast cycling and stable performance of these cells are attributed to the formation of robust, flexible, and tough F-rich conductive SEI on the surface of the in situ-deposited Li by benefiting from the combined effect of the resting protocol and the concentrated electrolyte. A condescending understanding of the mechanism of SEI formation and material choice could facilitate the development of AFBs as future advanced energy storage devices.

  View details for DOI 10.1021/acsami.9b09551

  View details for PubMedID 31393118

• Site Activity and Population Engineering of NiRu-Layered Double Hydroxide Nanosheets Decorated with Silver Nanoparticles for Oxygen Evolution and Reduction Reactions ACS CATALYSIS Chala, S., Tsai, M., Su, W., Ibrahim, K., Duma, A., Yeh, M., Wen, C., Yu, C., Chan, T., Dai, H., Hwang, B. 2019; 9 (1): 117–29

  View details for DOI 10.1021/acscatal.8b03092

  View details for Web of Science ID 000455286600013

• Rechargeable aluminum batteries: effects of cations in ionic liquid electrolytes RSC ADVANCES Zhu, G., Angell, M., Pan, C., Lin, M., Chen, H., Huang, C., Lin, J., Achazi, A. J., Kaghazchi, P., Hwang, B., Dai, H. 2019; 9 (20): 11322–30

  View details for DOI 10.1039/c9ra00765b

  View details for Web of Science ID 000466756100035

• Stabilizing lithium into cross-stacked nanotube sheets with ultra-high specific capacity for lithium oxygen battery. Angewandte Chemie (International ed. in English) Ye, L., Liao, M., Sun, H., Yang, Y., Tang, C., Zhao, Y., Wang, L., Xu, Y., Zhang, L., Wang, B., Xu, F., Sun, X., Zhang, Y., Dai, H., Bruce, P. G., Peng, H. 2018

  Abstract

  Although lithium-oxygen batteries possess high theoretical energy density and are considered as promising candidates for the next-generation power systems, how to enhance the safety and cycling efficiency of the lithium anodes while maintaining the high energy storage capability remains difficult. Here, we overcome this challenge by cross-stacking aligned carbon nanotubes into porous networks for ultrahigh-capacity lithium anodes to afford high-performance lithium-oxygen batteries. The novel anode shows a reversible specific capacity of 3656 mAh/g, approaching the theoretical capacity of 3861 mAh/g of pure lithium. When this anode is employed for lithium-oxygen full batteries, the cycling stability is significantly enhanced owing to the dendrite-free morphology and stabilized solid electrolyte interface. This work presents a new pathway to high performance lithium-oxygen batteries towards practical applications by designing cross-stacked and aligned structures for one-dimensional conducting nanomaterials.

  View details for PubMedID 30575248

• Developing a Bright NIR-II Fluorophore with Fast Renal Excretion and Its Application in Molecular Imaging of Immune Checkpoint PD-L1 ADVANCED FUNCTIONAL MATERIALS Wan, H., Ma, H., Zhu, S., Wang, F., Tian, Y., Ma, R., Yang, Q., Hu, Z., Zhu, T., Wang, W., Ma, Z., Zhang, M., Zhong, Y., Sun, H., Liang, Y., Dai, H. 2018; 28 (50)

  View details for DOI 10.1002/adfm.201804956

  View details for Web of Science ID 000456421000014

• Developing a Bright NIR-II Fluorophore with Fast Renal Excretion and Its Application in Molecular Imaging of Immune Checkpoint PD-L1. Advanced functional materials Wan, H., Ma, H., Zhu, S., Wang, F., Tian, Y., Ma, R., Yang, Q., Hu, Z., Zhu, T., Wang, W., Ma, Z., Zhang, M., Zhong, Y., Sun, H., Liang, Y., Dai, H. 2018; 28 (50)

  Abstract

  Fluorescence imaging in the second near-infrared (NIR-II) window holds impressive advantages of enhanced penetration depth and improved signal-to-noise ratio. Bright NIR-II fluorophores with renal excretion ability and low tissue accumulation are favorable for in vivo molecular imaging applications as they can render the target-mediated molecular imaging process easily distinguishable. Here, a probe (anti-PD-L1-BGP6) comprising a fluorophore (IR-BGP6) covalently bonded to the programmed cell death ligand-1 monoclonal antibody (PD-L1 mAb) for molecular imaging of immune checkpoint PD-L1 (a targeting site upregulated in various tumors for cancer imaging) in the NIR-II window is reported. Through molecular optimization, the bright NIR-II fluorophore IR-BGP6 with fast renal excretion (≈91% excretion in general through urine within the first 10 h postinjection) is developed. The conjugate anti-PD-L1-BGP6 succeeds in profiling PD-L1 expression and realizes efficient noninvasive molecular imaging in vivo, achieving a tumor to normal tissue (T/NT) signal ratio as high as ≈9.5. Compared with the NIR-II fluorophore with high nonspecific tissue accumulation, IR-BGP6 derived PD-L1 imaging significantly enhances the molecular imaging performance, serving as a strong tool for potentially studying underlying mechanism of immunotherapy. The work provides rationales to design renal-excreted NIR-II fluorophores and illustrate their advantages for in vivo molecular imaging.

  View details for DOI 10.1002/adfm.201804956

  View details for PubMedID 31832053

  View details for PubMedCentralID PMC6907024

• The inaugural Nano Research Young Innovators (NR45) Award in nanobiotechnology NANO RESEARCH Gu, Z., Dai, H. 2018; 11 (10): 4931–35

  View details for DOI 10.1007/s12274-018-2208-4

  View details for Web of Science ID 000446423900001

• Near-Infrared IIb Fluorescence Imaging of Vascular Regeneration with Dynamic Tissue Perfusion Measurement and High Spatial Resolution ADVANCED FUNCTIONAL MATERIALS Ma, Z., Zhang, M., Yue, J., Alcazar, C., Zhong, Y., Doyle, T. C., Dai, H., Huang, N. F. 2018; 28 (36)

  View details for DOI 10.1002/adfm.201803417

  View details for Web of Science ID 000443375900026

• Near-Infrared IIb Fluorescence Imaging of Vascular Regeneration with Dynamic Tissue Perfusion Measurement and High Spatial Resolution. Advanced functional materials Ma, Z., Zhang, M., Yue, J., Alcazar, C., Zhong, Y., Doyle, T. C., Dai, H., Huang, N. F. 2018; 28 (36)

  Abstract

  Real-time optical imaging is a promising approach for visualizing in vivo hemodynamics and vascular structure in mice with experimentally induced peripheral arterial disease (PAD). We report the application of a novel fluorescence-based all-optical imaging approach in the near-infrared IIb (NIR-IIb, 1500-1700 nm emission) window, for imaging hindlimb microvasculature and blood perfusion in a mouse model of PAD. In phantom studies, lead sulfide/cadmium sulfide (PbS/CdS) quantum dots showed better retention of image clarity, in comparison with single-walled nanotube (SWNT) NIR-IIa (1000-1400nm) dye, at varying depths of penetration. When systemically injected to mice, PbS/CdS demonstrated improved clarity of the vasculature, compared to SWNTs, as well as higher spatial resolution than in vivo microscopic computed tomography. In a mouse model of PAD, NIR-IIb imaging of the ischemic hindlimb vasculature showed significant improvement in blood perfusion over the course of 10 days (P<0.05), as well as a significant increase in microvascular density over the first 7 days after induction of PAD. In conclusion, NIR-IIb imaging of PbS/CdS vascular contrast agent is a useful multi-functional imaging approach for high spatial resolution imaging of the microvasculature and quantification of blood perfusion recovery.

  View details for DOI 10.1002/adfm.201803417

  View details for PubMedID 31327961

  View details for PubMedCentralID PMC6640151

• Bright quantum dots emitting at 1,600 nm in the NIR-IIb window for deep tissue fluorescence imaging. Proceedings of the National Academy of Sciences of the United States of America Zhang, M., Yue, J., Cui, R., Ma, Z., Wan, H., Wang, F., Zhu, S., Zhou, Y., Kuang, Y., Zhong, Y., Pang, D., Dai, H. 2018; 115 (26): 6590–95

  Abstract

  With suppressed photon scattering and diminished autofluorescence, in vivo fluorescence imaging in the 1,500- to 1,700-nm range of the near-IR (NIR) spectrum (NIR-IIb window) can afford high clarity and deep tissue penetration. However, there has been a lack of NIR-IIb fluorescent probes with sufficient brightness and aqueous stability. Here, we present a bright fluorescent probe emitting at 1,600 nm based on core/shell lead sulfide/cadmium sulfide (CdS) quantum dots (CSQDs) synthesized in organic phase. The CdS shell plays a critical role of protecting the lead sulfide (PbS) core from oxidation and retaining its bright fluorescence through the process of amphiphilic polymer coating and transferring to water needed for imparting aqueous stability and compatibility. The resulting CSQDs with a branched PEG outer layer exhibited a long blood circulation half-life of 7 hours and enabled through-skin, real-time imaging of blood flows in mouse vasculatures at an unprecedented 60 frames per second (fps) speed by detecting 1,600-nm fluorescence under 808-nm excitation. It also allowed through-skin in vivo confocal 3D imaging of tumor vasculatures in mice with an imaging depth of 1.2 mm. The PEG-CSQDs accumulated in tumor effectively through the enhanced permeation and retention effect, affording a high tumor-to-normal tissue ratio up to 32 owing to the bright 1,600-nm emission and nearly zero autofluorescence background resulting from a large 800-nm Stoke's shift. The aqueous-compatible CSQDs are excreted through the biliary pathway without causing obvious toxicity effects, suggesting a useful class of 1,600-nm emitting probes for biomedical research.

  View details for PubMedID 29891702

• Bright quantum dots emitting at similar to 1,600 nm in the NIR-IIb window for deep tissue fluorescence imaging PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Zhang, M., Yue, J., Cui, R., Ma, Z., Wan, H., Wang, F., Zhu, S., Zhou, Y., Kuang, Y., Zhong, Y., Pang, D., Dai, H. 2018; 115 (26): 6590–95

  View details for DOI 10.1073/pnas.1806153115

  View details for Web of Science ID 000436245000050

• Molecular Cancer Imaging in the Second Near-Infrared Window Using a Renal-Excreted NIR-II Fluorophore-Peptide Probe ADVANCED MATERIALS Wang, W., Ma, Z., Zhu, S., Wan, H., Yue, J., Ma, H., Ma, R., Yang, Q., Wang, Z., Li, Q., Qian, Y., Yue, C., Wang, Y., Fan, L., Zhong, Y., Zhou, Y., Gao, H., Ruan, J., Hu, Z., Liang, Y., Dai, H. 2018; 30 (22): e1800106

  Abstract

  In vivo molecular imaging of tumors targeting a specific cancer cell marker is a promising strategy for cancer diagnosis and imaging guided surgery and therapy. While targeted imaging often relies on antibody-modified probes, peptides can afford targeting probes with small sizes, high penetrating ability, and rapid excretion. Recently, in vivo fluorescence imaging in the second near-infrared window (NIR-II, 1000-1700 nm) shows promise in reaching sub-centimeter depth with microscale resolution. Here, a novel peptide (named CP) conjugated NIR-II fluorescent probe is reported for molecular tumor imaging targeting a tumor stem cell biomarker CD133. The click chemistry derived peptide-dye (CP-IRT dye) probe afforded efficient in vivo tumor targeting in mice with a high tumor-to-normal tissue signal ratio (T/NT > 8). Importantly, the CP-IRT probes are rapidly renal excreted (≈87% excretion within 6 h), in stark contrast to accumulation in the liver for typical antibody-dye probes. Further, with NIR-II emitting CP-IRT probes, urethra of mice can be imaged fluorescently for the first time noninvasively through intact tissue. The NIR-II fluorescent, CD133 targeting imaging probes are potentially useful for human use in the clinic for cancer diagnosis and therapy.

  View details for PubMedID 29682821

• An operando X-ray diffraction study of chloroaluminate anion-graphite intercalation in aluminum batteries PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Pan, C., Yuan, C., Zhu, G., Zhang, Q., Huang, C., Lin, M., Angell, M., Hwang, B., Kaghazchi, P., Dai, H. 2018; 115 (22): 5670–75

  Abstract

  We investigated rechargeable aluminum (Al) batteries composed of an Al negative electrode, a graphite positive electrode, and an ionic liquid (IL) electrolyte at temperatures down to -40 °C. The reversible battery discharge capacity at low temperatures could be superior to that at room temperature. In situ/operando electrochemical and synchrotron X-ray diffraction experiments combined with theoretical modeling revealed stable AlCl4-/graphite intercalation up to stage 3 at low temperatures, whereas intercalation was reversible up to stage 4 at room temperature (RT). The higher-degree anion/graphite intercalation at low temperatures affords rechargeable Al battery with higher discharge voltage (up to 2.5 V, a record for Al battery) and energy density. A remarkable cycle life of >20,000 cycles at a rate of 6C (10 minutes charge time) was achievable for Al battery operating at low temperatures, corresponding to a >50-year battery life if charged/discharged once daily.

  View details for PubMedID 29760096

• Robust and conductive Magneli Phase Ti4O7 decorated on 3D-nanoflower NiRu-LDH as high-performance oxygen reduction electrocatalyst NANO ENERGY Ibrahim, K., Su, W., Tsai, M., Chala, S., Kahsay, A., Yeh, M., Chen, H., Duma, A., Dai, H., Hwang, B. 2018; 47: 309–15

  View details for DOI 10.1016/j.nanoen.2018.03.017

  View details for Web of Science ID 000430057000032

• 3D NIR-II Molecular Imaging Distinguishes Targeted Organs with High-Performance NIR-II Bioconjugates ADVANCED MATERIALS Zhu, S., Herraiz, S., Yue, J., Zhang, M., Wan, H., Yang, Q., Ma, Z., Wang, Y., He, J., Antaris, A. L., Zhong, Y., Diao, S., Feng, Y., Zhou, Y., Yu, K., Hong, G., Liang, Y., Hsueh, A. J., Dai, H. 2018; 30 (13): e1705799

  Abstract

  Greatly reduced scattering in the second near-infrared (NIR-II) region (1000-1700 nm) opens up many new exciting avenues of bioimaging research, yet NIR-II fluorescence imaging is mostly implemented by using nontargeted fluorophores or wide-field imaging setups, limiting the signal-to-background ratio and imaging penetration depth due to poor specific binding and out-of-focus signals. A newly developed high-performance NIR-II bioconjugate enables targeted imaging of a specific organ in the living body with high quality. Combined with a home-built NIR-II confocal set-up, the enhanced imaging technique allows 900 µm-deep 3D organ imaging without tissue clearing techniques. Bioconjugation of two hormones to nonoverlapping NIR-II fluorophores facilitates two-color imaging of different receptors, demonstrating unprecedented multicolor live molecular imaging across the NIR-II window. This deep tissue imaging of specific receptors in live animals allows development of noninvasive molecular imaging of multifarious models of normal and neoplastic organs in vivo, beyond the traditional visible to NIR-I range. The developed NIR-II fluorescence microscopy will become a powerful imaging technique for deep tissue imaging without any physical sectioning or clearing treatment of the tissue.

  View details for PubMedID 29446156

  View details for PubMedCentralID PMC5931222

• A bright organic NIR-II nanofluorophore for three-dimensional imaging into biological tissues NATURE COMMUNICATIONS Wan, H., Yue, J., Zhu, S., Uno, T., Zhang, X., Yang, Q., Yu, K., Hong, G., Wang, J., Li, L., Ma, Z., Gao, H., Zhong, Y., Su, J., Antaris, A. L., Xia, Y., Luo, J., Liang, Y., Dai, H. 2018; 9: 1171

  Abstract

  Fluorescence imaging of biological systems in the second near-infrared (NIR-II, 1000-1700 nm) window has shown promise of high spatial resolution, low background, and deep tissue penetration owing to low autofluorescence and suppressed scattering of long wavelength photons. Here we develop a bright organic nanofluorophore (named p-FE) for high-performance biological imaging in the NIR-II window. The bright NIR-II >1100 nm fluorescence emission from p-FE affords non-invasive in vivo tracking of blood flow in mouse brain vessels. Excitingly, p-FE enables one-photon based, three-dimensional (3D) confocal imaging of vasculatures in fixed mouse brain tissue with a layer-by-layer imaging depth up to ~1.3 mm and sub-10 µm high spatial resolution. We also perform in vivo two-color fluorescence imaging in the NIR-II window by utilizing p-FE as a vasculature imaging agent emitting between 1100 and 1300 nm and single-walled carbon nanotubes (CNTs) emitting above 1500 nm to highlight tumors in mice.

  View details for PubMedID 29563581

• Donor Engineering for NIR-II Molecular Fluorophores with Enhanced Fluorescent Performance JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Yang, Q., Hu, Z., Zhu, S., Ma, R., Ma, H., Ma, Z., Wan, H., Zhu, T., Jiang, Z., Liu, W., Jiao, L., Sun, H., Liang, Y., Dai, H. 2018; 140 (5): 1715–24

  Abstract

  Organic fluorophores have been widely used for biological imaging in the visible and the first near-infrared windows. However, their application in the second near-infrared window (NIR-II, 1000-1700 nm) is still limited mainly due to low fluorescence quantum yields (QYs). Here, we explore molecular engineering on the donor unit to develop high performance NIR-II fluorophores. The fluorophores are constructed by a shielding unit-donor(s)-acceptor-donor(s)-shielding unit structure. Thiophene is introduced as the second donor connected to the shielding unit, which can increase the conjugation length and red-shift the fluorescence emission. Alkyl thiophene is employed as the first donor connected to the acceptor unit. The bulky and hydrophobic alkyl thiophene donor affords larger distortion of the conjugated backbone and fewer interactions with water molecules compared to other donor units studied before. The molecular fluorophore IR-FTAP with octyl thiophene as the first donor and thiophene as the second donor exhibits fluorescence emission peaked at 1048 nm with a QY of 5.3% in aqueous solutions, one of the highest for molecular NIR-II fluorophore reported so far. Superior temporal and spatial resolutions have been demonstrated with IR-FTAP fluorophore for NIR-II imaging of the blood vessels of a mouse hindlimb.

  View details for PubMedID 29337545

• Identification of the physical origin behind disorder, heterogeneity, and reconstruction and their correlation with the photoluminescence lifetime in hybrid perovskite thin films JOURNAL OF MATERIALS CHEMISTRY A Berhe, T., Cheng, J., Su, W., Pan, C., Tsai, M., Chen, H., Yang, Z., Tan, H., Chen, C., Yeh, M., Tamirat, A., Huang, S., Chen, L., Lee, J., Liao, Y., Sargent, E. H., Dai, H., Hwang, B. 2017; 5 (39): 21002–15

  View details for DOI 10.1039/c7ta04615d

  View details for Web of Science ID 000412800300054

• A high quantum yield molecule-protein complex fluorophore for near-infrared II imaging NATURE COMMUNICATIONS Antaris, A. L., Chen, H., Diao, S., Ma, Z., Zhang, Z., Zhu, S., Wang, J., Lozano, A. X., Fan, Q., Chew, L., Zhu, M., Cheng, K., Hong, X., Dai, H., Cheng, Z. 2017; 8

  Abstract

  Fluorescence imaging in the second near-infrared window (NIR-II) allows visualization of deep anatomical features with an unprecedented degree of clarity. NIR-II fluorophores draw from a broad spectrum of materials spanning semiconducting nanomaterials to organic molecular dyes, yet unfortunately all water-soluble organic molecules with >1,000 nm emission suffer from low quantum yields that have limited temporal resolution and penetration depth. Here, we report tailoring the supramolecular assemblies of protein complexes with a sulfonated NIR-II organic dye (CH-4T) to produce a brilliant 110-fold increase in fluorescence, resulting in the highest quantum yield molecular fluorophore thus far. The bright molecular complex allowed for the fastest video-rate imaging in the second NIR window with ∼50-fold reduced exposure times at a fast 50 frames-per-second (FPS) capable of resolving mouse cardiac cycles. In addition, we demonstrate that the NIR-II molecular complexes are superior to clinically approved ICG for lymph node imaging deep within the mouse body.

  View details for DOI 10.1038/ncomms15269

  View details for Web of Science ID 000401626200001

  View details for PubMedID 28524850

• Live imaging of follicle stimulating hormone receptors in gonads and bones using near infrared II fluorophore CHEMICAL SCIENCE Feng, Y., Zhu, S., Antaris, A. L., Chen, H., Xiao, Y., Lu, X., Jiang, L., Diao, S., Yu, K., Wang, Y., Herraiz, S., Yue, J., Hong, X., Hong, G., Cheng, Z., Dai, H., Hsueh, A. J. 2017; 8 (5): 3703-3711

  Abstract

  In vivo imaging of hormone receptors provides the opportunity to visualize target tissues under hormonal control in live animals. Detecting longer-wavelength photons in the second near-infrared window (NIR-II, 1000-1700 nm) region affords reduced photon scattering in tissues accompanied by lower autofluorescence, leading to higher spatial resolution at up to centimeter tissue penetration depths. Here, we report the conjugation of a small molecular NIR-II fluorophore CH1055 to a follicle stimulating hormone (FSH-CH) for imaging ovaries and testes in live mice. After exposure to FSH-CH, specific NIR-II signals were found in cultured ovarian granulosa cells containing FSH receptors. Injection of FSH-CH allowed live imaging of ovarian follicles and testicular seminiferous tubules in female and male adult mice, respectively. Using prepubertal mice, NIR-II signals were detected in ovaries containing only preantral follicles. Resolving earlier controversies regarding the expression of FSH receptors in cultured osteoclasts, we detected for the first time specific FSH receptor signals in bones in vivo. The present imaging of FSH receptors in live animals using a ligand-conjugated NIR-II fluorophore with low cell toxicity and rapid clearance allows the development of non-invasive molecular imaging of diverse hormonal target cells in vivo.

  View details for DOI 10.1039/c6sc04897h

  View details for Web of Science ID 000400553000048

  View details for PubMedCentralID PMC5465568

• Live imaging of follicle stimulating hormone receptors in gonads and bones using near infrared II fluorophore. Chemical science Feng, Y., Zhu, S., Antaris, A. L., Chen, H., Xiao, Y., Lu, X., Jiang, L., Diao, S., Yu, K., Wang, Y., Herraiz, S., Yue, J., Hong, X., Hong, G., Cheng, Z., Dai, H., Hsueh, A. J. 2017; 8 (5): 3703-3711

  Abstract

  In vivo imaging of hormone receptors provides the opportunity to visualize target tissues under hormonal control in live animals. Detecting longer-wavelength photons in the second near-infrared window (NIR-II, 1000-1700 nm) region affords reduced photon scattering in tissues accompanied by lower autofluorescence, leading to higher spatial resolution at up to centimeter tissue penetration depths. Here, we report the conjugation of a small molecular NIR-II fluorophore CH1055 to a follicle stimulating hormone (FSH-CH) for imaging ovaries and testes in live mice. After exposure to FSH-CH, specific NIR-II signals were found in cultured ovarian granulosa cells containing FSH receptors. Injection of FSH-CH allowed live imaging of ovarian follicles and testicular seminiferous tubules in female and male adult mice, respectively. Using prepubertal mice, NIR-II signals were detected in ovaries containing only preantral follicles. Resolving earlier controversies regarding the expression of FSH receptors in cultured osteoclasts, we detected for the first time specific FSH receptor signals in bones in vivo. The present imaging of FSH receptors in live animals using a ligand-conjugated NIR-II fluorophore with low cell toxicity and rapid clearance allows the development of non-invasive molecular imaging of diverse hormonal target cells in vivo.

  View details for DOI 10.1039/c6sc04897h

  View details for PubMedID 28626555

  View details for PubMedCentralID PMC5465568

• Diagnosis of Zika virus infection on a nanotechnology platform. Nature medicine Zhang, B., Pinsky, B. A., Ananta, J. S., Zhao, S., Arulkumar, S., Wan, H., Sahoo, M. K., Abeynayake, J., Waggoner, J. J., Hopes, C., Tang, M., Dai, H. 2017

  Abstract

  We developed a multiplexed assay on a plasmonic-gold platform for measuring IgG and IgA antibodies and IgG avidity against both Zika virus (ZIKV) and dengue virus (DENV) infections. In contrast to IgM cross-reactivity, IgG and IgA antibodies against ZIKV nonstructural protein 1 (NS1) antigen were specific to ZIKV infection, and IgG avidity revealed recent ZIKV infection and past DENV-2 infection in patients in dengue-endemic regions. This assay could enable specific diagnosis of ZIKV infection over other flaviviral infections.

  View details for DOI 10.1038/nm.4302

  View details for PubMedID 28263312

• Validation of IgG, IgM multiplex plasmonic gold platform in French clinical cohorts for the serodiagnosis and follow-up of Toxoplasma gondii infection. Diagnostic microbiology and infectious disease Pomares, C., Zhang, B., Arulkumar, S., Gonfrier, G., Marty, P., Zhao, S., Cheng, S., Tang, M., Dai, H., Montoya, J. G. 2017; 87 (3): 213-218

  Abstract

  We report the use of the multiplexed T. gondii IgG, IgM test on plasmonic gold (pGOLD) platform in the setting of T. gondii infection by analyzing 244 sera from Nice, France (seroconversion, chronically infected, non-infected and newborns serum samples). Results were compared with commercial tests for the detection of IgG and IgM and their overall clinical final interpretation of a complete serological profile. The IgG and IgM test results on the platform were in agreement in, respectively, 95% and 93% with the commercial kits. When comparing with the overall clinical interpretation of the serological profile, the agreement reached 99.5% and 97.7% for IgG and IgM, respectively. This innovative pGOLD platform allows detection of both IgG and IgM simultaneously with only ~1 microliter of serum. The multiplexed IgG/IgM test on pGOLD platform is a strong candidate for its use in the massive screening programs for toxoplasmosis during pregnancy.

  View details for DOI 10.1016/j.diagmicrobio.2016.09.001

  View details for PubMedID 28040304

• Advanced rechargeable aluminium ion battery with a high-quality natural graphite cathode NATURE COMMUNICATIONS Wang, D., Wei, C., Lin, M., Pan, C., Chou, H., Chen, H., Gong, M., Wu, Y., Yuan, C., Angell, M., Hsieh, Y., Chen, Y., Wen, C., Chen, C., Hwang, B., Chen, C., Dai, H. 2017; 8

  Abstract

  Recently, interest in aluminium ion batteries with aluminium anodes, graphite cathodes and ionic liquid electrolytes has increased; however, much remains to be done to increase the cathode capacity and to understand details of the anion-graphite intercalation mechanism. Here, an aluminium ion battery cell made using pristine natural graphite flakes achieves a specific capacity of ∼110 mAh g(-1) with Coulombic efficiency ∼98%, at a current density of 99 mA g(-1) (0.9 C) with clear discharge voltage plateaus (2.25-2.0 V and 1.9-1.5 V). The cell has a capacity of 60 mAh g(-1) at 6 C, over 6,000 cycles with Coulombic efficiency ∼ 99%. Raman spectroscopy shows two different intercalation processes involving chloroaluminate anions at the two discharging plateaus, while C-Cl bonding on the surface, or edges of natural graphite, is found using X-ray absorption spectroscopy. Finally, theoretical calculations are employed to investigate the intercalation behaviour of choloraluminate anions in the graphite electrode.

  View details for DOI 10.1038/ncomms14283

  View details for Web of Science ID 000393751900001

  View details for PubMedID 28194027

  View details for PubMedCentralID PMC5316828

• High Coulombic efficiency aluminum-ion battery using an AlCl3-urea ionic liquid analog electrolyte PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Angell, M., Pan, C., Rong, Y., Yuan, C., Lin, M., Hwang, B., Dai, H. 2017; 114 (5): 834-839

  Abstract

  In recent years, impressive advances in harvesting renewable energy have led to a pressing demand for the complimentary energy storage technology. Here, a high Coulombic efficiency (∼99.7%) Al battery is developed using earth-abundant aluminum as the anode, graphite as the cathode, and a cheap ionic liquid analog electrolyte made from a mixture of AlCl3 and urea in a 1.3:1 molar ratio. The battery displays discharge voltage plateaus around 1.9 and 1.5 V (average discharge = 1.73 V) and yielded a specific cathode capacity of ∼73 mAh g(-1) at a current density of 100 mA g(-1) (∼1.4 C). High Coulombic efficiency over a range of charge-discharge rates and stability over ∼150-200 cycles was easily demonstrated. In situ Raman spectroscopy clearly showed chloroaluminate anion intercalation/deintercalation of graphite (positive electrode) during charge-discharge and suggested the formation of a stage 2 graphite intercalation compound when fully charged. Raman spectroscopy and NMR suggested the existence of AlCl4(-), Al2Cl7(-) anions and [AlCl2·(urea)n](+) cations in the AlCl3/urea electrolyte when an excess of AlCl3 was present. Aluminum deposition therefore proceeded through two pathways, one involving Al2Cl7(-) anions and the other involving [AlCl2·(urea)n](+) cations. This battery is a promising prospect for a future high-performance, low-cost energy storage device.

  View details for DOI 10.1073/pnas.1619795114

  View details for Web of Science ID 000393196300041

  View details for PubMedID 28096353

  View details for PubMedCentralID PMC5293044

• Molecular imaging of biological systems with a clickable dye in the broad 800-to 1,700-nm near-infrared window PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Zhu, S., Yang, Q., Antaris, A. L., Yue, J., Ma, Z., Wang, H., Huang, W., Wan, H., Wang, J., Diao, S., Zhang, B., Li, X., Zhong, Y., Yu, K., Hong, G., Luo, J., Liang, Y., Dai, H. 2017; 114 (5): 962-967

  Abstract

  Fluorescence imaging multiplicity of biological systems is an area of intense focus, currently limited to fluorescence channels in the visible and first near-infrared (NIR-I; ∼700-900 nm) spectral regions. The development of conjugatable fluorophores with longer wavelength emission is highly desired to afford more targeting channels, reduce background autofluorescence, and achieve deeper tissue imaging depths. We have developed NIR-II (1,000-1,700 nm) molecular imaging agents with a bright NIR-II fluorophore through high-efficiency click chemistry to specific molecular antibodies. Relying on buoyant density differences during density gradient ultracentrifugation separations, highly pure NIR-II fluorophore-antibody conjugates emitting ∼1,100 nm were obtained for use as molecular-specific NIR-II probes. This facilitated 3D staining of ∼170-μm histological brain tissues sections on a home-built confocal microscope, demonstrating multicolor molecular imaging across both the NIR-I and NIR-II windows (800-1,700 nm).

  View details for DOI 10.1073/pnas.1617990114

  View details for PubMedID 28096386

• High Coulombic efficiency aluminum-ion battery using an AlCl3-urea ionic liquid analog electrolyte PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Angell, M., Pan, C., Rong, Y., Yuan, C., Lin, M., Hwang, B., Dai, H. 2017; 114 (5): 834-839

  Abstract

  In recent years, impressive advances in harvesting renewable energy have led to a pressing demand for the complimentary energy storage technology. Here, a high Coulombic efficiency (∼99.7%) Al battery is developed using earth-abundant aluminum as the anode, graphite as the cathode, and a cheap ionic liquid analog electrolyte made from a mixture of AlCl3 and urea in a 1.3:1 molar ratio. The battery displays discharge voltage plateaus around 1.9 and 1.5 V (average discharge = 1.73 V) and yielded a specific cathode capacity of ∼73 mAh g(-1) at a current density of 100 mA g(-1) (∼1.4 C). High Coulombic efficiency over a range of charge-discharge rates and stability over ∼150-200 cycles was easily demonstrated. In situ Raman spectroscopy clearly showed chloroaluminate anion intercalation/deintercalation of graphite (positive electrode) during charge-discharge and suggested the formation of a stage 2 graphite intercalation compound when fully charged. Raman spectroscopy and NMR suggested the existence of AlCl4(-), Al2Cl7(-) anions and [AlCl2·(urea)n](+) cations in the AlCl3/urea electrolyte when an excess of AlCl3 was present. Aluminum deposition therefore proceeded through two pathways, one involving Al2Cl7(-) anions and the other involving [AlCl2·(urea)n](+) cations. This battery is a promising prospect for a future high-performance, low-cost energy storage device.

  View details for DOI 10.1073/pnas.1619795114

  View details for Web of Science ID 000393196300041

  View details for PubMedID 28096353

  View details for PubMedCentralID PMC5293044

• Rational Design of Molecular Fluorophores for Biological Imaging in the NIR-II Window. Advanced materials Yang, Q., Ma, Z., Wang, H., Zhou, B., Zhu, S., Zhong, Y., Wang, J., Wan, H., Antaris, A., Ma, R., Zhang, X., Yang, J., Zhang, X., Sun, H., Liu, W., Liang, Y., Dai, H. 2017

  Abstract

  A new design for second near-infrared window (NIR-II) molecular fluorophores based on a shielding unit-donor-acceptor-donor-shielding unit (S-D-A-D-S) structure is reported. With 3,4-ethylenedioxy thiophene as the donor and fluorene as the shielding unit, the best performance fluorophores IR-FE and IR-FEP exhibit an emission quantum yield of 31% in toluene and 2.0% in water, respectively, representing the brightest organic dyes in NIR-II region reported so far.

  View details for DOI 10.1002/adma.201605497

  View details for PubMedID 28117499

• Boosting the down-shifting luminescence of rare-earth nanocrystals for biological imaging beyond 1500 nm. Nature communications Zhong, Y. n., Ma, Z. n., Zhu, S. n., Yue, J. n., Zhang, M. n., Antaris, A. L., Yuan, J. n., Cui, R. n., Wan, H. n., Zhou, Y. n., Wang, W. n., Huang, N. F., Luo, J. n., Hu, Z. n., Dai, H. n. 2017; 8 (1): 737

  Abstract

  In vivo fluorescence imaging in the near-infrared region between 1500-1700 nm (NIR-IIb window) affords high spatial resolution, deep-tissue penetration, and diminished auto-fluorescence due to the suppressed scattering of long-wavelength photons and large fluorophore Stokes shifts. However, very few NIR-IIb fluorescent probes exist currently. Here, we report the synthesis of a down-conversion luminescent rare-earth nanocrystal with cerium doping (Er/Ce co-doped NaYbF4 nanocrystal core with an inert NaYF4 shell). Ce doping is found to suppress the up-conversion pathway while boosting down-conversion by ~9-fold to produce bright 1550 nm luminescence under 980 nm excitation. Optimization of the inert shell coating surrounding the core and hydrophilic surface functionalization minimize the luminescence quenching effect by water. The resulting biocompatible, bright 1550 nm emitting nanoparticles enable fast in vivo imaging of blood vasculature in the mouse brain and hindlimb in the NIR-IIb window with short exposure time of 20 ms for rare-earth based probes.Fluorescence imaging in the near-infrared window between 1500-1700 nm (NIR-IIb window) offers superior spatial resolution and tissue penetration depth, but few NIR-IIb probes exist. Here, the authors synthesize rare earth down-converting nanocrystals as promising fluorescent probes for in vivo imaging in this spectral region.

  View details for PubMedID 28963467

  View details for PubMedCentralID PMC5622117

• Proteoliposome-based full-length ZnT8 self-antigen for type 1 diabetes diagnosis on a plasmonic platform. Proceedings of the National Academy of Sciences of the United States of America Wan, H. n., Merriman, C. n., Atkinson, M. A., Wasserfall, C. H., Mcgrail, K. M., Liang, Y. n., Fu, D. n., Dai, H. n. 2017; 114 (38): 10196–201

  Abstract

  Identified as a major biomarker for type 1 diabetes (T1D) diagnosis, zinc transporter 8 autoantibody (ZnT8A) has shown promise for staging disease risk and disease diagnosis. However, existing assays for ZnT8 autoantibody (ZnT8A) are limited to detection by soluble domains of ZnT8, owing to difficulties in maintaining proper folding of a full-length ZnT8 protein outside its native membrane environment. Through a combined bioengineering and nanotechnology approach, we have developed a proteoliposome-based full-length ZnT8 self-antigen (full-length ZnT8 proteoliposomes; PLR-ZnT8) for efficient detection of ZnT8A on a plasmonic gold chip (pGOLD). The protective lipid matrix of proteoliposomes improved the proper folding and structural stability of full-length ZnT8, helping PLR-ZnT8 immobilized on pGOLD (PLR-ZnT8/pGOLD) achieve high-affinity capture of ZnT8A from T1D sera. Our PLR-ZnT8/pGOLD exhibited efficient ZnT8A detection for T1D diagnosis with ∼76% sensitivity and ∼97% specificity (n = 307), superior to assays based on detergent-solubilized full-length ZnT8 and the C-terminal domain of ZnT8. Multiplexed assays using pGOLD were also developed for simultaneous detection of ZnT8A, islet antigen 2 autoantibody, and glutamic acid decarboxylase autoantibody for diagnosing T1D.

  View details for PubMedID 28874568

• Direct Evidence for Coupled Surface and Concentration Quenching Dynamics in Lanthanide-Doped Nanocrystals. Journal of the American Chemical Society Johnson, N. J., He, S. n., Diao, S. n., Chan, E. M., Dai, H. n., Almutairi, A. n. 2017; 139 (8): 3275–82

  Abstract

  Luminescence quenching at high dopant concentrations generally limits the dopant concentration to less than 1-5 mol% in lanthanide-doped materials, and this remains a major obstacle in designing materials with enhanced efficiency/brightness. In this work, we provide direct evidence that the major quenching process at high dopant concentrations is the energy migration to the surface (i.e., surface quenching) as opposed to the common misconception of cross-relaxation between dopant ions. We show that after an inert epitaxial shell growth, erbium (Er3+) concentrations as high as 100 mol% in NaY(Er)F4/NaLuF4 core/shell nanocrystals enhance the emission intensity of both upconversion and downshifted luminescence across different excitation wavelengths (980, 800, and 658 nm), with negligible concentration quenching effects. Our results highlight the strong coupling of concentration and surface quenching effects in colloidal lanthanide-doped nanocrystals, and that inert epitaxial shell growth can overcome concentration quenching. These fundamental insights into the photophysical processes in heavily doped nanocrystals will give rise to enhanced properties not previously thought possible with compositions optimized in bulk.

  View details for PubMedID 28169535

• Near-infrared fluorophores for biomedical imaging NATURE BIOMEDICAL ENGINEERING Hong, G., Antaris, A. L., Dai, H. 2017; 1 (1)

  View details for DOI 10.1038/s41551-016-0010

  View details for Web of Science ID 000418850600010

• Autoantibody profiling on a plasmonic nano-gold chip for the early detection of hypertensive heart disease. Proceedings of the National Academy of Sciences of the United States of America Li, X. n., Kuznetsova, T. n., Cauwenberghs, N. n., Wheeler, M. n., Maecker, H. n., Wu, J. C., Haddad, F. n., Dai, H. n. 2017; 114 (27): 7089–94

  Abstract

  The role of autoimmunity in cardiovascular (CV) diseases has been increasingly recognized. Autoimmunity is most commonly examined by the levels of circulating autoantibodies in clinical practices. Measurement of autoantibodies remains, however, challenging because of the deficiency of reproducible, sensitive, and standardized assays. The lack of multiplexed assays also limits the potential to identify a CV-specific autoantibody profile. To overcome these challenges, we developed a nanotechnology-based plasmonic gold chip for autoantibody profiling. This approach allowed simultaneous detection of 10 CV autoantibodies targeting the structural myocardial proteins, the neurohormonal regulatory proteins, the vascular proteins, and the proteins associated with apoptosis and coagulation. Autoantibodies were measured in four groups of participants across the continuum of hypertensive heart diseases. We observed higher levels of all 10 CV autoantibodies in hypertensive subjects (n= 77) compared with healthy participants (n= 30), and the autoantibodies investigated were related to each other, forming a highly linked network. In addition, we established that autoantibodies to troponin I, annexin-A5, and beta 1-adrenegic receptor best discriminated hypertensive subjects with adverse left ventricular (LV) remodeling or dysfunction (n= 49) from hypertensive subjects with normal LV structure and function (n= 28). By further linking these three significant CV autoantibodies to the innate and growth factors, we revealed a positive but weak association between autoantibodies to troponin I and proinflammatory cytokine IL-18. Overall, we demonstrated that this platform can be used to evaluate autoantibody profiles in hypertensive subjects at risk for heart failure.

  View details for PubMedID 28630342

• A novel quantitative microarray antibody capture (Q-MAC) assay identifies an extremely high HDV prevalence amongst HBV infected Mongolians. Hepatology Chen, X., Oidovsambuu, O., Liu, P., Grosely, R., Elazar, M., Winn, V. D., Fram, B., Boa, Z., Dai, H., Dashtseren, B., Yagaanbuyant, D., Genden, Z., Dashdorj, N., Bungert, A., Dashdorj, N., Glenn, J. S. 2016

  Abstract

  Hepatitis delta virus (HDV) causes the most severe form of human viral hepatitis. HDV requires a hepatitis B virus (HBV) co-infection to provide HDV with HBV surface antigen envelope proteins. The net effect of HDV is to make the underlying HBV disease worse, including higher rates of hepatocellular carcinoma (HCC). Accurate assessments of current HDV prevalence have been hampered by the lack of readily available and reliable quantitative assays, combined with the absence of an FDA-approved therapy. We sought to develop a convenient assay for accurately screening populations and to use this assay to determine HDV prevalence in a population with abnormally high rates of HCC. We developed a high throughput quantitative microarray antibody capture (Q-MAC) assay for anti-HDV IgG wherein recombinant HDV delta antigen is printed by microarray on slides coated with a noncontinuous, nanostructured plasmonic gold film, enabling quantitative fluorescent detection of anti-HDV antibody in small aliquots of patient serum. This assay was then used to screen all HBV-infected patients identified in a large randomly selected cohort designed to represent the Mongolian population. We identified two quantitative thresholds of captured antibody that were 100% predictive of the sample either being positive on standard western blot, or harboring HDV RNA detectable by qPCR, respectively. Subsequent screening of the HBV-positive cohort revealed that a remarkable 57% were RNA positive and an additional 4% were positive on western blot alone.The Q-MAC assay's unique performance characteristics make it ideal for population screening. Its application to the Mongolian HBsAg+ population reveals an apparent ∼60% prevalence of HDV co-infection amongst these HBV-infected Mongolian subjects, which may help explain the extraordinarily high rate of HCC in Mongolia. This article is protected by copyright. All rights reserved.

  View details for DOI 10.1002/hep.28957

  View details for PubMedID 27880976

• High Performance, Multiplexed Lung Cancer Biomarker Detection on a Plasmonic Gold Chip ADVANCED FUNCTIONAL MATERIALS Liu, B., Li, Y., Wan, H., Wang, L., Xu, W., Zhu, S., Liang, Y., Zhang, B., Lou, J., Dai, H., Qian, K. 2016; 26 (44): 7994-8002

  View details for DOI 10.1002/adfm.201603547

  View details for Web of Science ID 000388171100006

• 3D Graphitic Foams Derived from Chloroaluminate Anion Intercalation for Ultrafast Aluminum-Ion Battery. Advanced materials Wu, Y., Gong, M., Lin, M., Yuan, C., Angell, M., Huang, L., Wang, D., Zhang, X., Yang, J., Hwang, B., Dai, H. 2016; 28 (41): 9218-9222

  Abstract

  A 3D graphitic foam vertically aligned graphitic structure and a low density of defects is derived through chloroaluminate anion intercalation of graphite followed by thermal expansion and electrochemical hydrogen evolution. Such aligned graphitic structure affords excellent Al-ion battery characteristics with a discharge capacity of ≈60 mA h g(-1) under a high charge and discharge current density of 12 000 mA g(-1) over ≈4000 cycles.

  View details for DOI 10.1002/adma.201602958

  View details for PubMedID 27571346

• Facile Synthesis of [101]-Oriented Rutile TiO2 Nanorod Array on FTO Substrate with a Tunable Anatase-Rutile Heterojunction for Efficient Solar Water Splitting ACS SUSTAINABLE CHEMISTRY & ENGINEERING Sutiono, H., Tripathi, A. M., Chen, H., Chen, C., Su, W., Chen, L., Dai, H., Hwang, B. 2016; 4 (11): 5963-5971

  View details for DOI 10.1021/acssuschemeng.6b01066

  View details for Web of Science ID 000387428700019

• Hybrid anisotropic nanostructures for dual-modal cancer imaging and image-guided chemo-thermo therapies. Biomaterials Zhang, R., Cheng, K., Antaris, A. L., Ma, X., Yang, M., Ramakrishnan, S., Liu, G., Lu, A., Dai, H., Tian, M., Cheng, Z. 2016; 103: 265-277

  Abstract

  The multimodality theranostic system, which can integrate two or more different therapeutic modalities and multimodal imaging agents into a nanoentity, shows great promising prospects for the cancer treatment. Herein, we developed an efficient and novel strategy to synthesize hybrid anisotropic nanoparticles (HANs) with intrinsic multimodal theranostic capability [chemotherapy, photothermal therapy, magnetic resonance imaging (MRI), and photoacoustic imaging (PAI)]. For the first time, under the guidance of MRI and PAI, the chemotherapy and thermotherapy induced by administration of multifunctional hybrid nanoprobes were applied simultaneously to the treatment of colon cancer-bearing mice in vivo.

  View details for DOI 10.1016/j.biomaterials.2016.06.063

  View details for PubMedID 27394161

  View details for PubMedCentralID PMC4970737

• Traumatic Brain Injury Imaging in the Second Near-Infrared Window with a Molecular Fluorophore. Advanced materials Zhang, X., Wang, H., Antaris, A. L., Li, L., Diao, S., Ma, R., Nguyen, A., Hong, G., Ma, Z., Wang, J., Zhu, S., Castellano, J. M., Wyss-Coray, T., Liang, Y., Luo, J., Dai, H. 2016; 28 (32): 6872-6879

  Abstract

  Traumatic brain injury (TBI) is a leading cause of death and disability worldwide. A bright, renal-excreted, and biocompatible near-infrared II fluorophore for in vivo imaging of TBI is designed. A transient hypoperfusion in the injured cerebral region, followed by fluorophore leakage, is observed. NIR-II fluorophores can provide noninvasive assessment of TBI.

  View details for DOI 10.1002/adma.201600706

  View details for PubMedID 27253071

• IN VIVO VASCULAR IMAGING OF TRAUMATIC BRAIN INJURY IN THE SECOND NEAR-INFRARED WINDOW Zhang, X., Wang, H., Antaris, A., Li, L., Diao, S., Ma, R., Nguyen, A., Hong, G., Ma, Z., Wang, J., Zhu, S., Castellano, J., Wyss-Coray, T., Liang, Y., Luo, J., Dai, H. MARY ANN LIEBERT, INC. 2016: A48

  View details for Web of Science ID 000378336200127

• Multiplexed Anti-Toxoplasma IgG, IgM, and IgA Assay on Plasmonic Gold Chips: towards Making Mass Screening Possible with Dye Test Precision JOURNAL OF CLINICAL MICROBIOLOGY Li, X., Pomares, C., Gonfrier, G., Koh, B., Zhu, S., Gong, M., Montoya, J. G., Dai, H. 2016; 54 (7): 1726-1733

  Abstract

  Toxoplasmosis is an infection caused by the protozoan parasite Toxoplasma gondii that can lead to severe sequelae in the fetus during pregnancy. Definitive serologic diagnosis of the infection during gestation is made mostly by detecting T. gondii-specific antibodies, including IgG and IgM, individually in a single serum sample by using commercially available kits. The IgA test is used by some laboratories as an additional marker of acute infection. Most of the commercial tests have failed to reach 100% correlation with the reference method, the Sabin-Feldman dye test for the detection of Toxoplasma IgG antibodies. For Toxoplasma IgM and IgA antibodies, there is no reference method and their evaluation is done by comparing the results of one assay to those of another. There is a need for multiplexed assay platforms, as the serological diagnosis of T. gondii infection does not rely on the detection of a single Ig subtype. Here we describe the development of a plasmonic gold chip with vast fluorescence enhancement in the near-infrared region for simultaneous detection of IgG, IgM, and IgA antibodies against T. gondii in an ∼1-μl serum or whole-blood sample. When 168 samples were tested on this platform, IgG antibody detection sensitivity, specificity, positive predictive value (PPV), and negative predictive value (NPV) were all 100%. IgM antibody detection achieved 97.6% sensitivity and 96.9% specificity with a 90.9% PPV and a 99.2% NPV. Thus, the nanoscience-based plasmonic gold platform enables a high-performance, low-cost, multiplexed assay requiring ultrasmall blood volumes, paving the way for the implementation of universal screening for toxoplasmosis infection during gestation.

  View details for DOI 10.1128/JCM.00913-16

  View details for PubMedID 27008879

• A small-molecule dye for NIR-II imaging NATURE MATERIALS Antaris, A. L., Chen, H., Cheng, K., Sun, Y., Hong, G., Qu, C., Diao, S., Deng, Z., Hu, X., Zhang, B., Zhang, X., Yaghi, O. K., Alamparambil, Z. R., Hong, X., Cheng, Z., Dai, H. 2016; 15 (2): 235-?

  Abstract

  Fluorescent imaging of biological systems in the second near-infrared window (NIR-II) can probe tissue at centimetre depths and achieve micrometre-scale resolution at depths of millimetres. Unfortunately, all current NIR-II fluorophores are excreted slowly and are largely retained within the reticuloendothelial system, making clinical translation nearly impossible. Here, we report a rapidly excreted NIR-II fluorophore (∼90% excreted through the kidneys within 24 h) based on a synthetic 970-Da organic molecule (CH1055). The fluorophore outperformed indocyanine green (ICG)-a clinically approved NIR-I dye-in resolving mouse lymphatic vasculature and sentinel lymphatic mapping near a tumour. High levels of uptake of PEGylated-CH1055 dye were observed in brain tumours in mice, suggesting that the dye was detected at a depth of ∼4 mm. The CH1055 dye also allowed targeted molecular imaging of tumours in vivo when conjugated with anti-EGFR Affibody. Moreover, a superior tumour-to-background signal ratio allowed precise image-guided tumour-removal surgery.

  View details for DOI 10.1038/NMAT4476

  View details for Web of Science ID 000368766100030

• A small-molecule dye for NIR-II imaging. Nature materials Antaris, A. L., Chen, H., Cheng, K., Sun, Y., Hong, G., Qu, C., Diao, S., Deng, Z., Hu, X., Zhang, B., Zhang, X., Yaghi, O. K., Alamparambil, Z. R., Hong, X., Cheng, Z., Dai, H. 2016; 15 (2): 235-42

  Abstract

  Fluorescent imaging of biological systems in the second near-infrared window (NIR-II) can probe tissue at centimetre depths and achieve micrometre-scale resolution at depths of millimetres. Unfortunately, all current NIR-II fluorophores are excreted slowly and are largely retained within the reticuloendothelial system, making clinical translation nearly impossible. Here, we report a rapidly excreted NIR-II fluorophore (∼90% excreted through the kidneys within 24 h) based on a synthetic 970-Da organic molecule (CH1055). The fluorophore outperformed indocyanine green (ICG)-a clinically approved NIR-I dye-in resolving mouse lymphatic vasculature and sentinel lymphatic mapping near a tumour. High levels of uptake of PEGylated-CH1055 dye were observed in brain tumours in mice, suggesting that the dye was detected at a depth of ∼4 mm. The CH1055 dye also allowed targeted molecular imaging of tumours in vivo when conjugated with anti-EGFR Affibody. Moreover, a superior tumour-to-background signal ratio allowed precise image-guided tumour-removal surgery.

  View details for DOI 10.1038/nmat4476

  View details for PubMedID 26595119

• A mini review on nickel-based electrocatalysts for alkaline hydrogen evolution reaction NANO RESEARCH Gong, M., Wang, D., Chen, C., Hwang, B., Dai, H. 2016; 9 (1): 28-46

  View details for DOI 10.1007/s12274-015-0965-x

  View details for Web of Science ID 000371797800003

• In Vivo Fluorescence Imaging in the Second Near-Infrared Window Using Carbon Nanotubes IN VIVO FLUORESCENCE IMAGING: METHODS AND PROTOCOLS Hong, G., Dai, H., Bai, M. 2016; 1444: 167–81

  Abstract

  In vivo fluorescence imaging in the second near-infrared window (NIR-II window, 1000-1700 nm) is a powerful imaging technique that emerged in recent years. This imaging tool allows for noninvasive, deep-tissue visualization and interrogation of anatomical features and functions with improved imaging resolution and contrast at greater tissue penetration depths than traditional fluorescence imaging. Here, we present the detailed protocol for conducting NIR-II fluorescence imaging in live animals, including the procedures for preparation of biocompatible and NIR-II fluorescent carbon nanotube solution, live animal administration and NIR-II fluorescence image acquisition.

  View details for PubMedID 27283426

• Visible to Near-Infrared Fluorescence Enhanced Cellular Imaging on Plasmonic Gold Chips. Small Koh, B., Li, X., Zhang, B., Yuan, B., Lin, Y., Antaris, A. L., Wan, H., Gong, M., Yang, J., Zhang, X., Liang, Y., Dai, H. 2016; 12 (4): 457-465

  Abstract

  Rapid and sensitive detections of a variety of surface and intracellular proteins, nucleic acids, and other cellular biomarkers are important to elucidating biological signaling pathways and to devising disease diagnostics and therapeutics. Here, sensitive imaging and detection of cellular proteins on fluorescence-enhancing, nanostructured plasmonic gold (pGold) chips is presented. Imaging of fluorescently labeled cellular biomarkers on pGold is enhanced by 2-30-fold in the visible to near infrared (NIR) range of ≈500-900 nm. The high fluorescence enhancement of >700 nm significantly improves the dynamic range and signal/background ratios of NIR imaging, allowing high-performance multicolor imaging in the visible-NIR range using high quantum yield (QY) visible dyes and lower QY NIR fluorophores. Further, multiple cellular proteins of single cells of various cell types can be detected through microarraying of cells, useful for potentially hundreds and thousands different types of cells assayed on a single chip down to small cell numbers. This work suggests a simple, high throughput, high sensitivity, and multiplexed single-cell analysis method on fluorescence enhancing plasmonic substrates in the entire visible to NIR window.

  View details for DOI 10.1002/smll.201502182

  View details for PubMedID 26663862

• Single Chirality (6,4) Single-Walled Carbon Nanotubes for Fluorescence Imaging with Silicon Detectors SMALL Antaris, A. L., Yaghi, O. K., Hong, G., Diao, S., Zhang, B., Yang, J., Chew, L., Dai, H. 2015; 11 (47): 6325-6330

  Abstract

  Postsynthetic single-walled carbon nanotube (SWCNT) sorting methods such as density gradient ultracentrifugation, gel chromatography, and electrophoresis have all been inspired by established biochemistry separation techniques designed to separate subcellular components. Biochemistry separation techniques have been refined to the degree that parameters such as pH, salt concentration, and temperature are necessary for a successful separation, yet these conditions are only now being applied to SWCNT separation methodologies. Slight changes in pH produce radically different behaviors of SWCNTs inside a density gradient, allowing for the facile separation of ultrahigh purity (6,4) SWCNTs from as-synthesized carbon nanotubes. The (6,4) SWCNTs are novel fluorophores emitting below ≈900 nm and can be easily detected with conventional silicon-based charge-coupled device detectors without the need for specialized InGaAs cameras. The (6,4) SWCNTs are used to demonstrate their potential as a clinically relevant NIR-I fluorescence stain for the immunohistochemical staining of cells and cancer tissue sections displaying high endothelial growth factor receptor levels.

  View details for DOI 10.1002/smll.201501530

  View details for Web of Science ID 000367916600010

• Single Chirality (6,4) Single-Walled Carbon Nanotubes for Fluorescence Imaging with Silicon Detectors. Small (Weinheim an der Bergstrasse, Germany) Antaris, A. L., Yaghi, O. K., Hong, G., Diao, S., Zhang, B., Yang, J., Chew, L., Dai, H. 2015; 11 (47): 6325-30

  Abstract

  Postsynthetic single-walled carbon nanotube (SWCNT) sorting methods such as density gradient ultracentrifugation, gel chromatography, and electrophoresis have all been inspired by established biochemistry separation techniques designed to separate subcellular components. Biochemistry separation techniques have been refined to the degree that parameters such as pH, salt concentration, and temperature are necessary for a successful separation, yet these conditions are only now being applied to SWCNT separation methodologies. Slight changes in pH produce radically different behaviors of SWCNTs inside a density gradient, allowing for the facile separation of ultrahigh purity (6,4) SWCNTs from as-synthesized carbon nanotubes. The (6,4) SWCNTs are novel fluorophores emitting below ≈900 nm and can be easily detected with conventional silicon-based charge-coupled device detectors without the need for specialized InGaAs cameras. The (6,4) SWCNTs are used to demonstrate their potential as a clinically relevant NIR-I fluorescence stain for the immunohistochemical staining of cells and cancer tissue sections displaying high endothelial growth factor receptor levels.

  View details for DOI 10.1002/smll.201501530

  View details for PubMedID 26529611

• Fluorescence Imaging In Vivo at Wavelengths beyond 1500 nm ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Diao, S., Blackburn, J. L., Hong, G., Antaris, A. L., Chang, J., Wu, J. Z., Zhang, B., Cheng, K., Kuo, C. J., Dai, H. 2015; 54 (49): 14758-14762

  Abstract

  Compared to imaging in the visible and near-infrared regions below 900 nm, imaging in the second near-infrared window (NIR-II, 1000-1700 nm) is a promising method for deep-tissue high-resolution optical imaging in vivo mainly owing to the reduced scattering of photons traversing through biological tissues. Herein, semiconducting single-walled carbon nanotubes with large diameters were used for in vivo fluorescence imaging in the long-wavelength NIR region (1500-1700 nm, NIR-IIb). With this imaging agent, 3-4 μm wide capillary blood vessels at a depth of about 3 mm could be resolved. Meanwhile, the blood-flow speeds in multiple individual vessels could be mapped simultaneously. Furthermore, NIR-IIb tumor imaging of a live mouse was explored. NIR-IIb imaging can be generalized to a wide range of fluorophores emitting at up to 1700 nm for high-performance in vivo optical imaging.

  View details for DOI 10.1002/anie.201507473

  View details for Web of Science ID 000367723400025

• Fluorescence Imaging In Vivo at Wavelengths beyond 1500 nm. Angewandte Chemie (International ed. in English) Diao, S., Blackburn, J. L., Hong, G., Antaris, A. L., Chang, J., Wu, J. Z., Zhang, B., Cheng, K., Kuo, C. J., Dai, H. 2015; 54 (49): 14758-62

  Abstract

  Compared to imaging in the visible and near-infrared regions below 900 nm, imaging in the second near-infrared window (NIR-II, 1000-1700 nm) is a promising method for deep-tissue high-resolution optical imaging in vivo mainly owing to the reduced scattering of photons traversing through biological tissues. Herein, semiconducting single-walled carbon nanotubes with large diameters were used for in vivo fluorescence imaging in the long-wavelength NIR region (1500-1700 nm, NIR-IIb). With this imaging agent, 3-4 μm wide capillary blood vessels at a depth of about 3 mm could be resolved. Meanwhile, the blood-flow speeds in multiple individual vessels could be mapped simultaneously. Furthermore, NIR-IIb tumor imaging of a live mouse was explored. NIR-IIb imaging can be generalized to a wide range of fluorophores emitting at up to 1700 nm for high-performance in vivo optical imaging.

  View details for DOI 10.1002/anie.201507473

  View details for PubMedID 26460151

• Energy Migration Engineering of Bright Rare-Earth Upconversion Nanoparticles for Excitation by Light-Emitting Diodes ADVANCED MATERIALS Zhong, Y., Rostami, I., Wang, Z., Dai, H., Hu, Z. 2015; 27 (41): 6418-?

  Abstract

  A novel Nd(3+) -sensitized upconversion nanoparticle (UCNP) that can be excited by near-infrared 740 nm light-emitting diode (LED) lamps with bright upconversion luminescence is designed. Yb(3+) ion distribution is engineered to increase the energy migration efficiency. The benefit of the novel LED-excited UCNPs is demonstrated by imaging of breast cancer cells and enabling an economic handheld semiquantitative visual measurement device.

  View details for DOI 10.1002/adma.201502272

  View details for Web of Science ID 000364343700016

• Energy Migration Engineering of Bright Rare-Earth Upconversion Nanoparticles for Excitation by Light-Emitting Diodes. Advanced materials (Deerfield Beach, Fla.) Zhong, Y., Rostami, I., Wang, Z., Dai, H., Hu, Z. 2015; 27 (41): 6418-22

  Abstract

  A novel Nd(3+) -sensitized upconversion nanoparticle (UCNP) that can be excited by near-infrared 740 nm light-emitting diode (LED) lamps with bright upconversion luminescence is designed. Yb(3+) ion distribution is engineered to increase the energy migration efficiency. The benefit of the novel LED-excited UCNPs is demonstrated by imaging of breast cancer cells and enabling an economic handheld semiquantitative visual measurement device.

  View details for DOI 10.1002/adma.201502272

  View details for PubMedID 26393770

• Highly active and durable methanol oxidation electrocatalyst based on the synergy of platinum-nickel hydroxide-graphene NATURE COMMUNICATIONS Huang, W., Wang, H., Zhou, J., Wang, J., Duchesne, P. N., Muir, D., Zhang, P., Han, N., Zhao, F., Zeng, M., Zhong, J., Jin, C., Li, Y., Lee, S., Dai, H. 2015; 6

  Abstract

  Active and durable electrocatalysts for methanol oxidation reaction are of critical importance to the commercial viability of direct methanol fuel cell technology. Unfortunately, current methanol oxidation electrocatalysts fall far short of expectations and suffer from rapid activity degradation. Here we report platinum-nickel hydroxide-graphene ternary hybrids as a possible solution to this long-standing issue. The incorporation of highly defective nickel hydroxide nanostructures is believed to play the decisive role in promoting the dissociative adsorption of water molecules and subsequent oxidative removal of carbonaceous poison on neighbouring platinum sites. As a result, the ternary hybrids exhibit exceptional activity and durability towards efficient methanol oxidation reaction. Under periodic reactivations, the hybrids can endure at least 500,000 s with negligible activity loss, which is, to the best of our knowledge, two to three orders of magnitude longer than all available electrocatalysts.

  View details for DOI 10.1038/ncomms10035

  View details for PubMedID 26602295

• Carbon Nanomaterials for Biological Imaging and Nanomedicinal Therapy CHEMICAL REVIEWS Hong, G., Diao, S., Antaris, A. L., Dai, H. 2015; 115 (19): 10816-10906

  View details for DOI 10.1021/acs.chemrev.5b00008

  View details for Web of Science ID 000363002300009

  View details for PubMedID 25997028

• Blending Cr2 O3 into a NiO-Ni Electrocatalyst for Sustained Water Splitting. Angewandte Chemie (International ed. in English) Gong, M., Zhou, W., Kenney, M. J., Kapusta, R., Cowley, S., Wu, Y., Lu, B., Lin, M., Wang, D., Yang, J., Hwang, B., Dai, H. 2015; 54 (41): 11989-11993

  Abstract

  The rising H2 economy demands active and durable electrocatalysts based on low-cost, earth-abundant materials for water electrolysis/photolysis. Here we report nanoscale Ni metal cores over-coated by a Cr2 O3 -blended NiO layer synthesized on metallic foam substrates. The Ni@NiO/Cr2 O3 triphase material exhibits superior activity and stability similar to Pt for the hydrogen-evolution reaction in basic solutions. The chemically stable Cr2 O3 is crucial for preventing oxidation of the Ni core, maintaining abundant NiO/Ni interfaces as catalytically active sites in the heterostructure and thus imparting high stability to the hydrogen-evolution catalyst. The highly active and stable electrocatalyst enables an alkaline electrolyzer operating at 20 mA cm(-2) at a voltage lower than 1.5 V, lasting longer than 3 weeks without decay. The non-precious metal catalysts afford a high efficiency of about 15 % for light-driven water splitting using GaAs solar cells.

  View details for DOI 10.1002/anie.201504815

  View details for PubMedID 26307213

• Biological imaging without autofluorescence in the second near-infrared region NANO RESEARCH Diao, S., Hong, G., Antaris, A. L., Blackburn, J. L., Cheng, K., Cheng, Z., Dai, H. 2015; 8 (9): 3027-3034

  View details for DOI 10.1007/s12274-015-0808-9

  View details for Web of Science ID 000361057000025

• Ultra-active water electrolysis with Ni-based catalysts Gong, M., Zhou, W., Dai, H. AMER CHEMICAL SOC. 2015

  View details for Web of Science ID 000432475504254

• Cytokine detection and simultaneous assessment of rheumatoid factor interference in human serum and synovial fluid using high-sensitivity protein arrays on plasmonic gold chips BMC BIOTECHNOLOGY Valentina, M., Jan, F., Peder, N. L., Bo, Z., Dai Hongjie, H. J., Pernille, K. 2015; 15

  Abstract

  Fluorescence-enhancing microarray on plasmonic gold film is an attractive alternative to traditional enzyme-linked immunosorbent assay (ELISA) for cytokine detection because of the increased sensitivity. The assay chemistry is similar to an ELISA sandwich assay, but owing to the gold substrate, cytokine measurements are 10 to 100 times more sensitive and can be multiplexed. Plasmonic protein microarrays are, as other immunoassays, affected by the presence of heterophilic antibodies and rheumatoid factor may lead to analytical errors with serious implications for patient care. Here, we present a plasmonic gold substrate protein microarray for high-sensitivity detection of cytokines with simultaneous assessment of rheumatoid factor interference on a single chip.Paired serum and synovial fluid samples from patients with rheumatoid arthritis (n = 18), osteoarthritis (n = 9) or healthy controls (n = 10) were arrayed on near-infrared fluorescence enhancing plasmonic gold chips spotted with cytokine-specific capture antibody and isotype control antibody. Possible rheumatoid factor interference was visualised by a non-specific signal from the isotype control antibody, and pre-treatment of samples with heat-aggregated animal IgG eliminated this background contamination. The platform was optimised using the cytokine IL-20. The protein microarray platform allowed for the detection of human IL-20 at levels <1 pg/ml with reliable IL-20 quantification over a 5-log dynamic range. Samples for which rheumatoid factor caused artefacts were identified and a method for eliminating rheumatoid factor interference was developed and validated. IL-20 protein levels were significantly higher in synovial fluid samples from patients with rheumatoid arthritis compared to osteoarthritis (p < 0.001), while serum levels of IL-20 did not differ between patients with rheumatoid arthritis, osteoarthritis or healthy controls.Using novel plasmonic gold chips, we developed a highly sensitive and accurate assay platform to detect lowly expressed cytokines in biological fluids, allowing for the elimination of rheumatoid factor interference in as little as 5 μl sample volume. The detection limit was below 1 pg/ml for IL-20 and linearity was achieved over a 5-log dynamic range. This technology is highly advantageous for cytokines where sensitivity or sample volume is critical or where assessment of rheumatoid factor interference needs addressed and eliminated.

  View details for DOI 10.1186/s12896-015-0186-0

  View details for Web of Science ID 000359337200002

  View details for PubMedID 26268325

  View details for PubMedCentralID PMC4535377

• Aligned-Braided Nanofibrillar Scaffold with Endothelial Cells Enhances Arteriogenesis. ACS nano Nakayama, K. H., Hong, G., Lee, J. C., Patel, J., Edwards, B., Zaitseva, T. S., Paukshto, M. V., Dai, H., Cooke, J. P., Woo, Y. J., Huang, N. F. 2015; 9 (7): 6900-6908

  Abstract

  The objective of this study was to enhance the angiogenic capacity of endothelial cells (ECs) using nanoscale signaling cues from aligned nanofibrillar scaffolds in the setting of tissue ischemia. Thread-like nanofibrillar scaffolds with porous structure were fabricated from aligned-braided membranes generated under shear from liquid crystal collagen solution. Human ECs showed greater outgrowth from aligned scaffolds than from nonpatterned scaffolds. Integrin α1 was in part responsible for the enhanced cellular outgrowth on aligned nanofibrillar scaffolds, as the effect was abrogated by integrin α1 inhibition. To test the efficacy of EC-seeded aligned nanofibrillar scaffolds in improving neovascularization in vivo, the ischemic limbs of mice were treated with EC-seeded aligned nanofibrillar scaffold; EC-seeded nonpatterned scaffold; ECs in saline; aligned nanofibrillar scaffold alone; or no treatment. After 14 days, laser Doppler blood spectroscopy demonstrated significant improvement in blood perfusion recovery when treated with EC-seeded aligned nanofibrillar scaffolds, in comparison to ECs in saline or no treatment. In ischemic hindlimbs treated with scaffolds seeded with human ECs derived from induced pluripotent stem cells (iPSC-ECs), single-walled carbon nanotube (SWNT) fluorophores were systemically delivered to quantify microvascular density after 28 days. Near infrared-II (NIR-II, 1000-1700 nm) imaging of SWNT fluorophores demonstrated that iPSC-EC-seeded aligned scaffolds group showed significantly higher microvascular density than the saline or cells groups. These data suggest that treatment with EC-seeded aligned nanofibrillar scaffolds improved blood perfusion and arteriogenesis, when compared to treatment with cells alone or scaffold alone, and have important implications in the design of therapeutic cell delivery strategies.

  View details for DOI 10.1021/acsnano.5b00545

  View details for PubMedID 26061869

• Aligned-Braided Nanofibrillar Scaffold with Endothelial Cells Enhances Arteriogenesis ACS NANO Nakayarna, K. H., Hong, G., Lee, J. C., Patel, J., Edwards, B., Zaitseva, T. S., Paukshto, M. V., Dai, H., Cooke, J. P., Woo, Y. J., Huang, N. F. 2015; 9 (7): 6900-6908

  Abstract

  The objective of this study was to enhance the angiogenic capacity of endothelial cells (ECs) using nanoscale signaling cues from aligned nanofibrillar scaffolds in the setting of tissue ischemia. Thread-like nanofibrillar scaffolds with porous structure were fabricated from aligned-braided membranes generated under shear from liquid crystal collagen solution. Human ECs showed greater outgrowth from aligned scaffolds than from nonpatterned scaffolds. Integrin α1 was in part responsible for the enhanced cellular outgrowth on aligned nanofibrillar scaffolds, as the effect was abrogated by integrin α1 inhibition. To test the efficacy of EC-seeded aligned nanofibrillar scaffolds in improving neovascularization in vivo, the ischemic limbs of mice were treated with EC-seeded aligned nanofibrillar scaffold; EC-seeded nonpatterned scaffold; ECs in saline; aligned nanofibrillar scaffold alone; or no treatment. After 14 days, laser Doppler blood spectroscopy demonstrated significant improvement in blood perfusion recovery when treated with EC-seeded aligned nanofibrillar scaffolds, in comparison to ECs in saline or no treatment. In ischemic hindlimbs treated with scaffolds seeded with human ECs derived from induced pluripotent stem cells (iPSC-ECs), single-walled carbon nanotube (SWNT) fluorophores were systemically delivered to quantify microvascular density after 28 days. Near infrared-II (NIR-II, 1000-1700 nm) imaging of SWNT fluorophores demonstrated that iPSC-EC-seeded aligned scaffolds group showed significantly higher microvascular density than the saline or cells groups. These data suggest that treatment with EC-seeded aligned nanofibrillar scaffolds improved blood perfusion and arteriogenesis, when compared to treatment with cells alone or scaffold alone, and have important implications in the design of therapeutic cell delivery strategies.

  View details for DOI 10.1021/acsnano.5b00545

  View details for Web of Science ID 000358823200027

• Diketopyrrolopyrrole (DPP)-Based Donor-Acceptor Polymers for Selective Dispersion of Large-Diameter Semiconducting Carbon Nanotubes SMALL Lei, T., Lai, Y., Hong, G., Wang, H., Hayoz, P., Weitz, R. T., Chen, C., Dai, H., Bao, Z. 2015; 11 (24): 2946-2954

  Abstract

  Low-bandgap diketopyrrolopyrrole (DPP)-based polymers are used for the selective dispersion of semiconducting single-walled carbon nanotubes (s-SWCNTs). Through rational molecular design to tune the polymer-SWCNT interactions, highly selective dispersions of s-SWCNTs with diameters mainly around 1.5 nm are achieved. The influences of the polymer alkyl side-chain substitution (i.e., branched vs linear side chains) on the dispersing yield and selectivity of s-SWCNTs are investigated. Introducing linear alkyl side chains allows increased polymer-SWCNT interactions through close π-π stacking and improved C-H-π interactions. This work demonstrates that polymer side-chain engineering is an effective method to modulate the polymer-SWCNT interactions and thereby affecting both critical parameters in dispersing yield and selectivity. Using these sorted s-SWCNTs, high-performance SWCNT network thin-film transistors are fabricated. The solution-deposited s-SWCNT transistors yield simultaneously high mobilities of 41.2 cm(2) V(-1) s(-1) and high on/off ratios of greater than 10(4) . In summary, low-bandgap DPP donor-acceptor polymers are a promising class of polymers for selective dispersion of large-diameter s-SWCNTs.

  View details for DOI 10.1002/smll.201403761

  View details for PubMedID 25711378

• Nickel-coated silicon photocathode for water splitting in alkaline electrolytes NANO RESEARCH Feng, J., Gong, M., Kenney, M. J., Wu, J. Z., Zhang, B., Li, Y., Dai, H. 2015; 8 (5): 1577-1583

  View details for DOI 10.1007/s12274-014-0643-4

  View details for Web of Science ID 000354625600013

• An ultrafast rechargeable aluminium-ion battery. Nature Lin, M., Gong, M., Lu, B., Wu, Y., Wang, D., Guan, M., Angell, M., Chen, C., Yang, J., Hwang, B., Dai, H. 2015; 520 (7547): 325-328

  Abstract

  The development of new rechargeable battery systems could fuel various energy applications, from personal electronics to grid storage. Rechargeable aluminium-based batteries offer the possibilities of low cost and low flammability, together with three-electron-redox properties leading to high capacity. However, research efforts over the past 30 years have encountered numerous problems, such as cathode material disintegration, low cell discharge voltage (about 0.55 volts; ref. 5), capacitive behaviour without discharge voltage plateaus (1.1-0.2 volts or 1.8-0.8 volts) and insufficient cycle life (less than 100 cycles) with rapid capacity decay (by 26-85 per cent over 100 cycles). Here we present a rechargeable aluminium battery with high-rate capability that uses an aluminium metal anode and a three-dimensional graphitic-foam cathode. The battery operates through the electrochemical deposition and dissolution of aluminium at the anode, and intercalation/de-intercalation of chloroaluminate anions in the graphite, using a non-flammable ionic liquid electrolyte. The cell exhibits well-defined discharge voltage plateaus near 2 volts, a specific capacity of about 70 mA h g(-1) and a Coulombic efficiency of approximately 98 per cent. The cathode was found to enable fast anion diffusion and intercalation, affording charging times of around one minute with a current density of ~4,000 mA g(-1) (equivalent to ~3,000 W kg(-1)), and to withstand more than 7,500 cycles without capacity decay.

  View details for DOI 10.1038/nature14340

  View details for PubMedID 25849777

• An ultrafast rechargeable aluminium-ion battery NATURE Lin, M., Gong, M., Lu, B., Wu, Y., Wang, D., Guan, M., Angell, M., Chen, C., Yang, J., Hwang, B., Dai, H. 2015; 520 (7547): 325-?

  Abstract

  The development of new rechargeable battery systems could fuel various energy applications, from personal electronics to grid storage. Rechargeable aluminium-based batteries offer the possibilities of low cost and low flammability, together with three-electron-redox properties leading to high capacity. However, research efforts over the past 30 years have encountered numerous problems, such as cathode material disintegration, low cell discharge voltage (about 0.55 volts; ref. 5), capacitive behaviour without discharge voltage plateaus (1.1-0.2 volts or 1.8-0.8 volts) and insufficient cycle life (less than 100 cycles) with rapid capacity decay (by 26-85 per cent over 100 cycles). Here we present a rechargeable aluminium battery with high-rate capability that uses an aluminium metal anode and a three-dimensional graphitic-foam cathode. The battery operates through the electrochemical deposition and dissolution of aluminium at the anode, and intercalation/de-intercalation of chloroaluminate anions in the graphite, using a non-flammable ionic liquid electrolyte. The cell exhibits well-defined discharge voltage plateaus near 2 volts, a specific capacity of about 70 mA h g(-1) and a Coulombic efficiency of approximately 98 per cent. The cathode was found to enable fast anion diffusion and intercalation, affording charging times of around one minute with a current density of ~4,000 mA g(-1) (equivalent to ~3,000 W kg(-1)), and to withstand more than 7,500 cycles without capacity decay.

  View details for DOI 10.1038/nature14340

  View details for Web of Science ID 000352974200033

  View details for PubMedID 25849777

• Highly Active and Stable Hybrid Catalyst of Cobalt-Doped FeS2 Nanosheets-Carbon Nanotubes for Hydrogen Evolution Reaction. Journal of the American Chemical Society Wang, D., Gong, M., Chou, H., Pan, C., Chen, H., Wu, Y., Lin, M., Guan, M., Yang, J., Chen, C., Wang, Y., Hwang, B., Chen, C., Dai, H. 2015; 137 (4): 1587-1592

  Abstract

  Hydrogen evolution reaction (HER) from water through electrocatalysis using cost-effective materials to replace precious Pt catalysts holds great promise for clean energy technologies. In this work we developed a highly active and stable catalyst containing Co doped earth abundant iron pyrite FeS(2) nanosheets hybridized with carbon nanotubes (Fe(1-x)CoxS(2)/CNT hybrid catalysts) for HER in acidic solutions. The pyrite phase of Fe(1-x)CoxS(2)/CNT was characterized by powder X-ray diffraction and absorption spectroscopy. Electrochemical measurements showed a low overpotential of ∼0.12 V at 20 mA/cm(2), small Tafel slope of ∼46 mV/decade, and long-term durability over 40 h of HER operation using bulk quantities of Fe(0.9)Co(0.1)S(2)/CNT hybrid catalysts at high loadings (∼7 mg/cm(2)). Density functional theory calculation revealed that the origin of high catalytic activity stemmed from a large reduction of the kinetic energy barrier of H atom adsorption on FeS(2) surface upon Co doping in the iron pyrite structure. It is also found that the high HER catalytic activity of Fe(0.9)Co(0.1)S(2) hinges on the hybridization with CNTs to impart strong heteroatomic interactions between CNT and Fe(0.9)Co(0.1)S(2). This work produces the most active HER catalyst based on iron pyrite, suggesting a scalable, low cost, and highly efficient catalyst for hydrogen generation.

  View details for DOI 10.1021/ja511572q

  View details for PubMedID 25588180

• Graphene nanoribbons under mechanical strain. Advanced materials Chen, C., Wu, J. Z., Lam, K. T., Hong, G., Gong, M., Zhang, B., Lu, Y., Antaris, A. L., Diao, S., Guo, J., Dai, H. 2015; 27 (2): 303-309

  Abstract

  Uniaxial strains are introduced into individual graphene nanoribbons (GNRs) with highly smooth edges to investigate the strain effects on Raman spectroscopic and electrical properties of GNRs. It is found that uniaxial strain downshifts the Raman G-band frequency of GNRs linearly and tunes their bandgap significantly in a non-monotonic manner. The strain engineering of GNRs is promising for potential electronics and photonics applications.

  View details for DOI 10.1002/adma.201403750

  View details for PubMedID 25355690

• A mini review of NiFe-based materials as highly active oxygen evolution reaction electrocatalysts NANO RESEARCH Gong, M., Dai, H. 2015; 8 (1): 23-39

  View details for DOI 10.1007/s12274-014-0591-z

  View details for Web of Science ID 000348200300002

• Top-Down Patterning and Self-Assembly for Regular Arrays of Semiconducting Single-Walled Carbon Nanotubes ADVANCED MATERIALS Wu, J., Antaris, A., Gong, M., Dai, H. 2014; 26 (35): 6151-?

  Abstract

  Highly pure semiconducting single-walled carbon nanotubes (SWNTs), sorted by density-gradient ultracentrifugation, undergo self-assembly using depletion attraction forces into rafts along lithographically defined patterns of narrow pitch (100 or 200 nm). The arrays demonstrate high pattern fidelity and channel filling, along with large-scale homogeneity. Field-effect transistors made from these arrays exhibit high performance at on/off ratios>1000.

  View details for DOI 10.1002/adma.201401108

  View details for Web of Science ID 000342148600015

• Top-down patterning and self-assembly for regular arrays of semiconducting single-walled carbon nanotubes. Advanced materials Wu, J., Antaris, A., Gong, M., Dai, H. 2014; 26 (35): 6151-6156

  Abstract

  Highly pure semiconducting single-walled carbon nanotubes (SWNTs), sorted by density-gradient ultracentrifugation, undergo self-assembly using depletion attraction forces into rafts along lithographically defined patterns of narrow pitch (100 or 200 nm). The arrays demonstrate high pattern fidelity and channel filling, along with large-scale homogeneity. Field-effect transistors made from these arrays exhibit high performance at on/off ratios>1000.

  View details for DOI 10.1002/adma.201401108

  View details for PubMedID 25047392

• Through-skull fluorescence imaging of the brain in a new near-infrared window NATURE PHOTONICS Hong, G., Diao, S., Chang, J., Antaris, A. L., Chen, C., Zhang, B., Zhao, S., Atochin, D. N., Huang, P. L., Andreasson, K. I., Kuo, C. J., Dai, H. 2014; 8 (9): 723-730

  Abstract

  To date, brain imaging has largely relied on X-ray computed tomography and magnetic resonance angiography with limited spatial resolution and long scanning times. Fluorescence-based brain imaging in the visible and traditional near-infrared regions (400-900 nm) is an alternative but currently requires craniotomy, cranial windows and skull thinning techniques, and the penetration depth is limited to 1-2 mm due to light scattering. Here, we report through-scalp and through-skull fluorescence imaging of mouse cerebral vasculature without craniotomy utilizing the intrinsic photoluminescence of single-walled carbon nanotubes in the 1.3-1.4 micrometre near-infrared window. Reduced photon scattering in this spectral region allows fluorescence imaging reaching a depth of >2 mm in mouse brain with sub-10 micrometre resolution. An imaging rate of ~5.3 frames/s allows for dynamic recording of blood perfusion in the cerebral vessels with sufficient temporal resolution, providing real-time assessment of blood flow anomaly in a mouse middle cerebral artery occlusion stroke model.

  View details for DOI 10.1038/NPHOTON.2014.166

  View details for Web of Science ID 000342600100016

  View details for PubMedCentralID PMC5026222

• Through-skull fluorescence imaging of the brain in a new near-infrared window. Nature photonics Hong, G., Diao, S., Chang, J., Antaris, A. L., Chen, C., Zhang, B., Zhao, S., Atochin, D. N., Huang, P. L., Andreasson, K. I., Kuo, C. J., Dai, H. 2014; 8 (9): 723-730

  Abstract

  To date, brain imaging has largely relied on X-ray computed tomography and magnetic resonance angiography with limited spatial resolution and long scanning times. Fluorescence-based brain imaging in the visible and traditional near-infrared regions (400-900 nm) is an alternative but currently requires craniotomy, cranial windows and skull thinning techniques, and the penetration depth is limited to 1-2 mm due to light scattering. Here, we report through-scalp and through-skull fluorescence imaging of mouse cerebral vasculature without craniotomy utilizing the intrinsic photoluminescence of single-walled carbon nanotubes in the 1.3-1.4 micrometre near-infrared window. Reduced photon scattering in this spectral region allows fluorescence imaging reaching a depth of >2 mm in mouse brain with sub-10 micrometre resolution. An imaging rate of ~5.3 frames/s allows for dynamic recording of blood perfusion in the cerebral vessels with sufficient temporal resolution, providing real-time assessment of blood flow anomaly in a mouse middle cerebral artery occlusion stroke model.

  View details for DOI 10.1038/nphoton.2014.166

  View details for PubMedID 27642366

  View details for PubMedCentralID PMC5026222

• Tumor Metastasis Inhibition by Imaging-Guided Photothermal Therapy with Single-Walled Carbon Nanotubes ADVANCED MATERIALS Liang, C., Diao, S., Wang, C., Gong, H., Liu, T., Hong, G., Shi, X., Dai, H., Liu, Z. 2014; 26 (32): 5646-?

  Abstract

  Multi-modal imaging guided photothermal therapy with single-walled carbon nanotubes affords effective destruction of primary tumors together with cancer cells in sentinel lymph nodes. This results in remarkably prolonged mouse survival compared to mice treated by elimination of only the primary tumor by either surgery or conventional photothermal therapy.

  View details for DOI 10.1002/adma.201401825

  View details for Web of Science ID 000340900800007

  View details for PubMedID 24924258

• Diketopyrrolopyrrole (DPP)-based donor-acceptor polymers for scalable and selective dispersion of large-diameter carbon nanotubes Lei, T., Lai, Y., Hong, G., Wang, H., Dai, H., Bao, Z. AMER CHEMICAL SOC. 2014

  View details for Web of Science ID 000349167405040

• Recent advances in zinc-air batteries CHEMICAL SOCIETY REVIEWS Li, Y., Dai, H. 2014; 43 (15): 5257-5275

  Abstract

  Zinc-air is a century-old battery technology but has attracted revived interest recently. With larger storage capacity at a fraction of the cost compared to lithium-ion, zinc-air batteries clearly represent one of the most viable future options to powering electric vehicles. However, some technical problems associated with them have yet to be resolved. In this review, we present the fundamentals, challenges and latest exciting advances related to zinc-air research. Detailed discussion will be organized around the individual components of the system - from zinc electrodes, electrolytes, and separators to air electrodes and oxygen electrocatalysts in sequential order for both primary and electrically/mechanically rechargeable types. The detrimental effect of CO2 on battery performance is also emphasized, and possible solutions summarized. Finally, other metal-air batteries are briefly overviewed and compared in favor of zinc-air.

  View details for DOI 10.1039/c4cs00015c

  View details for Web of Science ID 000339306800009

  View details for PubMedID 24926965

• A plasmonic chip for biomarker discovery and diagnosis of type 1 diabetes. Nature medicine Zhang, B., Kumar, R. B., Dai, H., Feldman, B. J. 2014; 20 (8): 948-953

  Abstract

  Type 1 diabetes (T1D) is an autoimmune disease, whereas type 2 diabetes (T2D) results from insulin resistance and beta cell dysfunction. Previously, the onset of these two separate diseases was easily distinguished, with children being most at risk for T1D and T2D occurring in overweight adults. However, the dramatic rise in obesity, coupled with the notable increase in T1D, has created a large overlap in these previously discrete patient populations. Delayed diagnosis of T1D can result in severe illness or death, and rapid diagnosis of T1D is critical for the efficacy of emerging therapies. However, attempts to apply next-generation platforms have been unsuccessful for detecting diabetes biomarkers. Here we describe the development of a plasmonic gold chip for near-infrared fluorescence-enhanced (NIR-FE) detection of islet cell-targeting autoantibodies. We demonstrate that this platform has high sensitivity and specificity for the diagnosis of T1D and can be used to discover previously unknown biomarkers of T1D.

  View details for DOI 10.1038/nm.3619

  View details for PubMedID 25038825

• Ultrathin WS2 Nanoflakes as a High-Performance Electrocatalyst for the Hydrogen Evolution Reaction ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Cheng, L., Huang, W., Gong, Q., Liu, C., Liu, Z., Li, Y., Dai, H. 2014; 53 (30): 7860-7863

  Abstract

  Much has been done to search for highly efficient and inexpensive electrocatalysts for the hydrogen evolution reaction (HER), which is critical to a range of electrochemical and photoelectrochemical processes. A new, high-temperature solution-phase method for the synthesis of ultrathin WS2 nanoflakes is now reported. The resulting product possesses monolayer thickness with dimensions in the nanometer range and abundant edges. These favorable structural features render the WS2 nanoflakes highly active and durable catalysts for the HER in acids. The catalyst exhibits a small HER overpotential of approximately 100 mV and a Tafel slope of 48 mV/decade. These ultrathin WS2 nanoflakes represent an attractive alternative to the precious platinum benchmark catalyst and rival MoS2 materials that have recently been heavily scrutinized for the electrocatalytic HER.

  View details for DOI 10.1002/anie.201402315

  View details for Web of Science ID 000339562400030

  View details for PubMedID 24838978

• Ultrafast fluorescence imaging in vivo with conjugated polymer fluorophores in the second near-infrared window NATURE COMMUNICATIONS Hong, G., Zou, Y., Antaris, A. L., Diao, S., Wu, D., Cheng, K., Zhang, X., Chen, C., Liu, B., He, Y., Wu, J. Z., Yuan, J., Zhang, B., Tao, Z., Fukunaga, C., Dai, H. 2014; 5

  Abstract

  In vivo fluorescence imaging in the second near-infrared window (1.0-1.7 μm) can afford deep tissue penetration and high spatial resolution, owing to the reduced scattering of long-wavelength photons. Here we synthesize a series of low-bandgap donor/acceptor copolymers with tunable emission wavelengths of 1,050-1,350 nm in this window. Non-covalent functionalization with phospholipid-polyethylene glycol results in water-soluble and biocompatible polymeric nanoparticles, allowing for live cell molecular imaging at >1,000 nm with polymer fluorophores for the first time. Importantly, the high quantum yield of the polymer allows for in vivo, deep-tissue and ultrafast imaging of mouse arterial blood flow with an unprecedented frame rate of >25 frames per second. The high time-resolution results in spatially and time resolved imaging of the blood flow pattern in cardiogram waveform over a single cardiac cycle (~200 ms) of a mouse, which has not been observed with fluorescence imaging in this window before.

  View details for DOI 10.1038/ncomms5206

  View details for Web of Science ID 000338839100002

• Ultrafast high-capacity NiZn battery with NiAlCo-layered double hydroxide ENERGY & ENVIRONMENTAL SCIENCE Gong, M., Li, Y., Zhang, H., Zhang, B., Zhou, W., Feng, J., Wang, H., Liang, Y., Fan, Z., Liu, J., Dai, H. 2014; 7 (6): 2025-2032

  View details for DOI 10.1039/c4ee00317a

  View details for Web of Science ID 000336831700026

• Ly108 expression distinguishes subsets of invariant NKT cells that help autoantibody production and secrete IL-21 from those that secrete IL-17 in lupus prone NZB/W mice. Journal of autoimmunity Tang, X., Zhang, B., Jarrell, J. A., Price, J. V., Dai, H., Utz, P. J., Strober, S. 2014; 50: 87-98

  Abstract

  Lupus is a systemic autoimmune disease characterized by anti-nuclear antibodies in humans and genetically susceptible NZB/W mice that can cause immune complex glomerulonephritis. T cells contribute to lupus pathogenesis by secreting pro-inflammatory cytokines such as IL-17, and by interacting with B cells and secreting helper factors such as IL-21 that promote production of IgG autoantibodies. In the current study, we determined whether purified NKT cells or far more numerous conventional non-NKT cells in the spleen of NZB/W female mice secrete IL-17 and/or IL-21 after TCR activation in vitro, and provide help for spontaneous IgG autoantibody production by purified splenic CD19(+) B cells. Whereas invariant NKT cells secreted large amounts of IL-17 and IL-21, and helped B cells, non-NKT cells did not. The subset of IL-17 secreting NZB/W NKT cells expressed the Ly108(lo)CD4(-)NK1.1(-) phenotype, whereas the IL-21 secreting subset expressed the Ly108(hi)CD4(+)NK1.1(-) phenotype and helped B cells secrete a variety of IgG anti-nuclear antibodies. α-galactocylceramide enhanced the helper activity of NZB/W and B6.Sle1b NKT cells for IgG autoantibody secretion by syngeneic B cells. In conclusion, different subsets of iNKT cells from mice with genetic susceptibility to lupus can contribute to pathogenesis by secreting pro-inflammatory cytokines and helping autoantibody production.

  View details for DOI 10.1016/j.jaut.2014.01.002

  View details for PubMedID 24508410

  View details for PubMedCentralID PMC4002579

• Near-infrared II fluorescence for imaging hindlimb vessel regeneration with dynamic tissue perfusion measurement. Circulation. Cardiovascular imaging Hong, G., Lee, J. C., Jha, A., Diao, S., Nakayama, K. H., Hou, L., Doyle, T. C., Robinson, J. T., Antaris, A. L., Dai, H., Cooke, J. P., Huang, N. F. 2014; 7 (3): 517-525

  Abstract

  Real-time vascular imaging that provides both anatomic and hemodynamic information could greatly facilitate the diagnosis of vascular diseases and provide accurate assessment of therapeutic effects. Here, we have developed a novel fluorescence-based all-optical method, named near-infrared II (NIR-II) fluorescence imaging, to image murine hindlimb vasculature and blood flow in an experimental model of peripheral arterial disease, by exploiting fluorescence in the NIR-II region (1000-1400 nm) of photon wavelengths.Because of the reduced photon scattering of NIR-II fluorescence compared with traditional NIR fluorescence imaging and thus much deeper penetration depth into the body, we demonstrated that the mouse hindlimb vasculature could be imaged with higher spatial resolution than in vivo microscopic computed tomography. Furthermore, imaging during 26 days revealed a significant increase in hindlimb microvascular density in response to experimentally induced ischemia within the first 8 days of the surgery (P<0.005), which was confirmed by histological analysis of microvascular density. Moreover, the tissue perfusion in the ischemic hindlimb could be quantitatively measured by the dynamic NIR-II method, revealing the temporal kinetics of blood flow recovery that resembled microbead-based blood flowmetry and laser Doppler blood spectroscopy.The penetration depth of millimeters, high spatial resolution, and fast acquisition rate of NIR-II imaging make it a useful imaging tool for murine models of vascular disease.

  View details for DOI 10.1161/CIRCIMAGING.113.000305

  View details for PubMedID 24657826

• Near-Infrared II Fluorescence for Imaging Hindlimb Vessel Regeneration With Dynamic Tissue Perfusion Measurement. Circulation. Cardiovascular imaging Hong, G., Lee, J. C., Jha, A., Diao, S., Nakayama, K. H., Hou, L., Doyle, T. C., Robinson, J. T., Antaris, A. L., Dai, H., Cooke, J. P., Huang, N. F. 2014; 7 (3): 517-525

  Abstract

  Real-time vascular imaging that provides both anatomic and hemodynamic information could greatly facilitate the diagnosis of vascular diseases and provide accurate assessment of therapeutic effects. Here, we have developed a novel fluorescence-based all-optical method, named near-infrared II (NIR-II) fluorescence imaging, to image murine hindlimb vasculature and blood flow in an experimental model of peripheral arterial disease, by exploiting fluorescence in the NIR-II region (1000-1400 nm) of photon wavelengths.Because of the reduced photon scattering of NIR-II fluorescence compared with traditional NIR fluorescence imaging and thus much deeper penetration depth into the body, we demonstrated that the mouse hindlimb vasculature could be imaged with higher spatial resolution than in vivo microscopic computed tomography. Furthermore, imaging during 26 days revealed a significant increase in hindlimb microvascular density in response to experimentally induced ischemia within the first 8 days of the surgery (P<0.005), which was confirmed by histological analysis of microvascular density. Moreover, the tissue perfusion in the ischemic hindlimb could be quantitatively measured by the dynamic NIR-II method, revealing the temporal kinetics of blood flow recovery that resembled microbead-based blood flowmetry and laser Doppler blood spectroscopy.The penetration depth of millimeters, high spatial resolution, and fast acquisition rate of NIR-II imaging make it a useful imaging tool for murine models of vascular disease.

  View details for DOI 10.1161/CIRCIMAGING.113.000305

  View details for PubMedID 24657826

• Graphite Oxide Nanoparticles with Diameter Greater than 20 nm Are Biocompatible with Mouse Embryonic Stem Cells and Can Be Used in a Tissue Engineering System. Small Wang, I. E., Robinson, J. T., Do, G., Hong, G., Gould, D. R., Dai, H., Yang, P. C. 2014; 10 (8): 1479-1484

  Abstract

  Graphite oxide sheets demonstrate size-dependent uptake and toxicity towards embryonic stem cells. Graphite oxide sheets larger than 20 nm are biocompatible and can be safely used with mouse embryonic stem cells, while graphite oxide sheets smaller than 20 nm in diameter reduced cell proliferation and increased cell toxicity.

  View details for DOI 10.1002/smll.201303133

  View details for PubMedID 24376186

• Dependence of the Absorption and Optical Surface Plasmon Scattering of MoS2 Nanoparticles on Aspect Ratio, Size, and Media ACS NANO Yadgarov, L., Choi, C. L., Sedova, A., Cohen, A., Rosentsveig, R., Bar-Elli, O., Oron, D., Dai, H., Tenne, R. 2014; 8 (4): 3575-3583

  Abstract

  The optical and electronic properties of suspensions of inorganic fullerene-like nanoparticles of MoS2 are studied through light absorption and zeta-potential measurements and compared to those of the corresponding microscopic platelets. The total extinction measurements show that, in addition to excitonic peaks and the indirect band gap transition, a new peak is observed at 700-800 nm. This spectral peak has not been reported previously for MoS2. Comparison of the total extinction and decoupled absorption spectrum indicates that this peak largely originates from scattering. Furthermore, the dependence of this peak on nanoparticle size, shape, and surface charge, as well as solvent refractive index, suggests that this transition arises from a plasmon resonance.

  View details for DOI 10.1021/nn5000354

  View details for Web of Science ID 000334990600049

  View details for PubMedID 24669749

• Plasmonic micro-beads for fluorescence enhanced, multiplexed protein detection with flow cytometry CHEMICAL SCIENCE Zhang, B., Yang, J., Zou, Y., Gong, M., Chen, H., Hong, G., Antaris, A. L., Li, X., Liu, C., Chen, C., Dai, H. 2014; 5 (10): 4070-4075

  View details for DOI 10.1039/c4sc01206b

  View details for Web of Science ID 000341195100048

• Ultrafast fluorescence imaging in vivo with conjugated polymer fluorophores in the second near-infrared window. Nature communications Hong, G., Zou, Y., Antaris, A. L., Diao, S., Wu, D., Cheng, K., Zhang, X., Chen, C., Liu, B., He, Y., Wu, J. Z., Yuan, J., Zhang, B., Tao, Z., Fukunaga, C., Dai, H. 2014; 5: 4206-?

  Abstract

  In vivo fluorescence imaging in the second near-infrared window (1.0-1.7 μm) can afford deep tissue penetration and high spatial resolution, owing to the reduced scattering of long-wavelength photons. Here we synthesize a series of low-bandgap donor/acceptor copolymers with tunable emission wavelengths of 1,050-1,350 nm in this window. Non-covalent functionalization with phospholipid-polyethylene glycol results in water-soluble and biocompatible polymeric nanoparticles, allowing for live cell molecular imaging at >1,000 nm with polymer fluorophores for the first time. Importantly, the high quantum yield of the polymer allows for in vivo, deep-tissue and ultrafast imaging of mouse arterial blood flow with an unprecedented frame rate of >25 frames per second. The high time-resolution results in spatially and time resolved imaging of the blood flow pattern in cardiogram waveform over a single cardiac cycle (~200 ms) of a mouse, which has not been observed with fluorescence imaging in this window before.

  View details for DOI 10.1038/ncomms5206

  View details for PubMedID 24947309

• Nanoscale nickel oxide/nickel heterostructures for active hydrogen evolution electrocatalysis. Nature communications Gong, M., Zhou, W., Tsai, M., Zhou, J., Guan, M., Lin, M., Zhang, B., Hu, Y., Wang, D., Yang, J., Pennycook, S. J., Hwang, B., Dai, H. 2014; 5: 4695-?

  Abstract

  Active, stable and cost-effective electrocatalysts are a key to water splitting for hydrogen production through electrolysis or photoelectrochemistry. Here we report nanoscale nickel oxide/nickel heterostructures formed on carbon nanotube sidewalls as highly effective electrocatalysts for hydrogen evolution reaction with activity similar to platinum. Partially reduced nickel interfaced with nickel oxide results from thermal decomposition of nickel hydroxide precursors bonded to carbon nanotube sidewalls. The metal ion-carbon nanotube interactions impede complete reduction and Ostwald ripening of nickel species into the less hydrogen evolution reaction active pure nickel phase. A water electrolyzer that achieves ~20 mA cm(-2) at a voltage of 1.5 V, and which may be operated by a single-cell alkaline battery, is fabricated using cheap, non-precious metal-based electrocatalysts.

  View details for DOI 10.1038/ncomms5695

  View details for PubMedID 25146255

• Nanoscale nickel oxide/nickel heterostructures for active hydrogen evolution electrocatalysis. Nature communications Gong, M., Zhou, W., Tsai, M., Zhou, J., Guan, M., Lin, M., Zhang, B., Hu, Y., Wang, D., Yang, J., Pennycook, S. J., Hwang, B., Dai, H. 2014; 5: 4695-?

  Abstract

  Active, stable and cost-effective electrocatalysts are a key to water splitting for hydrogen production through electrolysis or photoelectrochemistry. Here we report nanoscale nickel oxide/nickel heterostructures formed on carbon nanotube sidewalls as highly effective electrocatalysts for hydrogen evolution reaction with activity similar to platinum. Partially reduced nickel interfaced with nickel oxide results from thermal decomposition of nickel hydroxide precursors bonded to carbon nanotube sidewalls. The metal ion-carbon nanotube interactions impede complete reduction and Ostwald ripening of nickel species into the less hydrogen evolution reaction active pure nickel phase. A water electrolyzer that achieves ~20 mA cm(-2) at a voltage of 1.5 V, and which may be operated by a single-cell alkaline battery, is fabricated using cheap, non-precious metal-based electrocatalysts.

  View details for DOI 10.1038/ncomms5695

  View details for PubMedID 25146255

• Fe-N bonding in a carbon nanotube-graphene complex for oxygen reduction: an XAS study PHYSICAL CHEMISTRY CHEMICAL PHYSICS Zhou, J., Duchesne, P. N., Hu, Y., Wang, J., Zhang, P., Li, Y., Regier, T., Dai, H. 2014; 16 (30): 15787-15791

  Abstract

  The electronic structure study of carbon nanotube-graphene complexes has been performed using comprehensive X-ray absorption spectroscopy (XAS) at Fe L- and K-edges, along with C, N and O K-edges. The results obtained from the study of an iron-containing carbon nanotube-graphene complex (NT-G) have been compared in great detail with those of an iron-free carbon nanotube-graphene complex (pNT-G) and iron phthalocyanine (FePc). It has been confirmed that complex-like Fe(3+) in a high spin state is the major iron component in NT-G. The C and N K-edge XANES further confirmed that Fe is very likely to be bonded to N in NT-G. This Fe-N species should be the active site for enhanced oxygen reduction reaction (ORR) activity in NT-G. A unique O K-edge X-ray absorption spectroscopic feature has been observed in NT-G, which might be caused by chemisorbed O2 on the Fe-N site. Such knowledge is important for the understanding of this specific complex, and the knowledge should benefit the rational design of other carbon/metal/nitrogen-containing ORR catalysts with further improved performance.

  View details for DOI 10.1039/c4cp01455c

  View details for Web of Science ID 000339628400006

  View details for PubMedID 24963799

• Self-assembly of semiconducting single-walled carbon nanotubes into dense, aligned rafts. Small Wu, J., Jiao, L., Antaris, A., Choi, C. L., Xie, L., Wu, Y., Diao, S., Chen, C., Chen, Y., Dai, H. 2013; 9 (24): 4142-4148

  Abstract

  Highly pure semiconducting single-walled carbon nanotubes (SWNTs) are separated from bulk materials and self-assembled into densely aligned rafts. Microscopy and spectroscopy reveals ∼100 SWNTs per micrometer within the rafts. Short channel field-effect transistors (FETs) from tens of purely semiconducting SWNTs within a submicrometer channel width achieve unprecedented on-currents (up to 121 μA) with high on/off ratios. The results demonstrate densely aligned semiconducting SWNTs for high-performance nanoelectronics.

  View details for DOI 10.1002/smll.201301547

  View details for PubMedID 23843273

• Self-Assembly of Semiconducting Single-Walled Carbon Nanotubes into Dense, Aligned Rafts SMALL Wu, J., Jiao, L., Antaris, A., Choi, C. L., Xie, L., Wu, Y., Diao, S., Chen, C., Chen, Y., Dai, H. 2013; 9 (24): 4142-4148

  View details for DOI 10.1002/smll.201301547

  View details for Web of Science ID 000328453300008

• Biological Imaging Using Nanoparticles of Small Organic Molecules with Fluorescence Emission at Wavelengths Longer than 1000 nm. Angewandte Chemie (International ed. in English) Tao, Z., Hong, G., Shinji, C., Chen, C., Diao, S., Antaris, A. L., Zhang, B., Zou, Y., Dai, H. 2013; 52 (49): 13002-13006

  Abstract

  Embedded in a polymer: A hydrophobic organic molecule that fluoresces in the near-infrared II (NIR-II) region was made water-soluble and biocompatible by its embedment in a polymer nanoparticle, which was then coated with hydrophilic poly(ethylene glycol) chains. The resulting nanoparticles exhibit bright fluorescence in the NIR-II window and high photostability in aqueous media and were used for in vivo imaging in mice.

  View details for DOI 10.1002/anie.201307346

  View details for PubMedID 24174264

• WS2 nanoflakes from nanotubes for electrocatalysis NANO RESEARCH Choi, C. L., Feng, J., Li, Y., Wu, J., Zak, A., Tenne, R., Dai, H. 2013; 6 (12): 921-928

  View details for DOI 10.1007/s12274-013-0369-8

  View details for Web of Science ID 000328899800007

• High-performance silicon photoanodes passivated with ultrathin nickel films for water oxidation. Science Kenney, M. J., Gong, M., Li, Y., Wu, J. Z., Feng, J., Lanza, M., Dai, H. 2013; 342 (6160): 836-840

  Abstract

  Silicon's sensitivity to corrosion has hindered its use in photoanode applications. We found that deposition of a ~2-nanometer nickel film on n-type silicon (n-Si) with its native oxide affords a high-performance metal-insulator-semiconductor photoanode for photoelectrochemical (PEC) water oxidation in both aqueous potassium hydroxide (KOH, pH = 14) and aqueous borate buffer (pH = 9.5) solutions. The Ni film acted as a surface protection layer against corrosion and as a nonprecious metal electrocatalyst for oxygen evolution. In 1 M aqueous KOH, the Ni/n-Si photoanodes exhibited high PEC activity with a low onset potential (~1.07 volts versus reversible hydrogen electrode), high photocurrent density, and durability. The electrode showed no sign of decay after ~80 hours of continuous PEC water oxidation in a mixed lithium borate-potassium borate electrolyte. The high photovoltage was attributed to a high built-in potential in a metal-insulator-semiconductor-like device with an ultrathin, incomplete screening Ni/NiO(x) layer from the electrolyte.

  View details for DOI 10.1126/science.1241327

  View details for PubMedID 24233719

• High-Performance Silicon Photoanodes Passivated with Ultrathin Nickel Films for Water Oxidation SCIENCE Kenney, M. J., Gong, M., Li, Y., Wu, J. Z., Feng, J., Lanza, M., Dai, H. 2013; 342 (6160): 836-840

  View details for DOI 10.1126/science.1241327

  View details for Web of Science ID 000326923000032

• HREM analysis of graphite-encapsulated metallic nanoparticles for possible medical applications. Ultramicroscopy Sinclair, R., Li, H., Madsen, S., Dai, H. 2013; 134: 167-174

  Abstract

  High resolution electron microscopy has been applied to study the structure of metallic nanoparticles. These have sparked considerable interest as contrast agents in the field of biological imaging, including in magnetic resonance imaging (MRI) and computed tomography (CT). Here, we describe a method of synthesizing sub-10nm superparamagnetic metal and alloy nanoparticles by reduction of metallic salts. Annealing at 900°C in a methane/hydrogen environment forms a thin graphitic-carbon shell which is expected to improve stability, biocompatibility, and functionalization. Subsequent high resolution electron microscopy verifies graphitization and allows for crystallographic analysis. Most particles consist of single crystals in the phase predicted for the bulk material at the annealing temperature. Electron energy loss spectroscopy, energy dispersive X-ray spectroscopy and lattice constant measurements show large variation in composition for alloy nanoparticles from a single synthesis. The magnetization relaxation time (T2) measurements demonstrate that Fe and AuFe nanoparticles compete with commercially available iron oxide MRI contrast agents. X-ray attenuation measurements of an AuFe alloy nanoparticle solution gave a relative radiodensity of 280 Hounsfield Units, demonstrating promise as a dual-purpose contrast agent in CT and MRI. Long term stability in an atmospheric environment was also tested, with no signs of corrosion or oxidation after several years of storage.

  View details for DOI 10.1016/j.ultramic.2013.05.006

  View details for PubMedID 23809196

• An advanced ni-fe layered double hydroxide electrocatalyst for water oxidation. Journal of the American Chemical Society Gong, M., Li, Y., Wang, H., Liang, Y., Wu, J. Z., Zhou, J., Wang, J., Regier, T., Wei, F., Dai, H. 2013; 135 (23): 8452-8455

  Abstract

  Highly active, durable, and cost-effective electrocatalysts for water oxidation to evolve oxygen gas hold a key to a range of renewable energy solutions, including water-splitting and rechargeable metal-air batteries. Here, we report the synthesis of ultrathin nickel-iron layered double hydroxide (NiFe-LDH) nanoplates on mildly oxidized multiwalled carbon nanotubes (CNTs). Incorporation of Fe into the nickel hydroxide induced the formation of NiFe-LDH. The crystalline NiFe-LDH phase in nanoplate form is found to be highly active for oxygen evolution reaction in alkaline solutions. For NiFe-LDH grown on a network of CNTs, the resulting NiFe-LDH/CNT complex exhibits higher electrocatalytic activity and stability for oxygen evolution than commercial precious metal Ir catalysts.

  View details for DOI 10.1021/ja4027715

  View details for PubMedID 23701670

• Biodistribution, pharmacokinetics and toxicology of Ag2S near-infrared quantum dots in mice BIOMATERIALS Zhang, Y., Zhang, Y., Hong, G., He, W., Zhou, K., Yang, K., Li, F., Chen, G., Liu, Z., Dai, H., Wang, Q. 2013; 34 (14): 3639-3646

  Abstract

  Ag2S quantum dots (QDs) have been demonstrated as a promising near-infrared II (NIR-II, 1.0-1.4 μm) emitting nanoprobe for in vivo imaging and detection. In this work, we carefully study the long-term in vivo biodistribution of Ag2S QDs functionalized with polyethylene glycol (PEG) and systematically examine the potential toxicity of Ag2S QDs over time. Our results show that PEGylated-Ag2S QDs are mainly accumulated in the reticuloendothelial system (RES) including liver and spleen after intravenous administration and can be gradually cleared, mostly by fecal excretion. PEGylated-Ag2S QDs do not cause appreciable toxicity at our tested doses (15 and 30 mg/kg) to the treated mice over a period of 2 months as evidenced by blood biochemistry, hematological analysis and histological examinations. Our work lays a solid foundation for further biomedical applications of Ag2S QDs as an important in vivo imaging agent in the NIR-II region.

  View details for DOI 10.1016/j.biomaterials.2013.01.089

  View details for Web of Science ID 000317534200010

  View details for PubMedID 23415643

• Chemical sorting, functionalization, and assembly of carbon nanotube for biological and nanoelectronics applications Dai, H. AMER CHEMICAL SOC. 2013

  View details for Web of Science ID 000324303604148

• Strongly coupled inorganic/nanocarbon hybrid materials for advanced electrocatalysis Dai, H. AMER CHEMICAL SOC. 2013

  View details for Web of Science ID 000323851304648

• Strongly coupled inorganic/graphitic-nanocarbon hybrid materials for energy storage Dai, H. AMER CHEMICAL SOC. 2013

  View details for Web of Science ID 000323851304717

• High-resolution, serial intravital microscopic imaging of nanoparticle delivery and targeting in a small animal tumor model NANO TODAY Smith, B. R., Zavaleta, C., Rosenberg, J., Tong, R., Ramunas, J., Liu, Z., Dai, H., Gambhir, S. S. 2013; 8 (2): 126-137

  View details for DOI 10.1016/j.nantod.2013.02.004

  View details for Web of Science ID 000319236400006

• High-resolution, serial intravital microscopic imaging of nanoparticle delivery and targeting in a small animal tumor model. Nano today Smith, B. R., Zavaleta, C., Rosenberg, J., Tong, R., Ramunas, J., Liu, Z., Dai, H., Gambhir, S. S. 2013; 8 (2)

  Abstract

  Nanoparticles are under active investigation for the detection and treatment of cancer. Yet our understanding of nanoparticle delivery to tumors is limited by our ability to observe the uptake process on its own scale in living subjects. We chose to study single-walled carbon nanotubes (SWNTs) because they exhibit among the highest levels of tumor uptake across the wide variety of available nanoparticles. We target them using RGD (arginine-glycine-aspartic acid) peptide which directs them to integrins overexpressed on tumor vasculature and on the surface of some tumor cells (e.g., U87MG as used here). We employ intravital microscopy (IVM) to quantitatively examine the spatiotemporal framework of targeted SWNT uptake in a murine tumor model. IVM provided a dynamic microscale window into nanoparticle circulation, binding to tumor blood vessels, extravasation, binding to tumor cells, and tumor retention. RGD-SWNTs bound to tumor vasculature significantly more than controls (P<0.0001). RGD-SWNTs extravasated similarly compared to control RAD-SWNTs, but post-extravasation we observed as RGD-SWNTs eventually bound to individual tumor cells significantly more than RAD-SWNTs (p<0.0001) over time. RGD-SWNTs and RAD-SWNTs displayed similar signal in tumor for a week, but over time their curves significantly diverged (p<0.001) showing increasing RGD-SWNTs relative to untargeted SWNTs. We uncovered the complex spatiotemporal interplay between these competing uptake mechanisms. Specific uptake was delimited to early (1-6 hours) and late (1-4 weeks) time-points, while non-specific uptake dominated from 6 hours to 1 week. Our analysis revealed critical, quantitative insights into the dynamic, multifaceted mechanisms implicated in ligand-targeted SWNT accumulation in tumor using real-time observation.

  View details for DOI 10.1016/j.nantod.2013.02.004

  View details for PubMedID 24273594

  View details for PubMedCentralID PMC3836612

• Ultra-Low Doses of Chirality Sorted (6,5) Carbon Nanotubes for Simultaneous Tumor Imaging and Photothermal Therapy ACS NANO Antaris, A. L., Robinson, J. T., Yaghi, O. K., Hong, G., Diao, S., Luong, R., Dai, H. 2013; 7 (4): 3644-3652

  Abstract

  Single-walled carbon nanotubes (SWCNTs) exhibit intrinsic fluorescence and strong optical absorption in the near-infrared (NIR) biological window (0.7-1.4 μm), rendering them ideal for in vivo imaging and photothermal therapy. Advances in SWCNT sorting have led to improved nanoelectronics and are promising for nanomedicine. To date, SWCNTs used in vivo consist of heterogeneous mixtures of nanotubes and only a small subset of chirality nanotubes fluoresces or heats under a NIR laser. Here, we demonstrate that separated (6,5) SWCNTs exchanged into a biocompatible surfactant, C18-PMH-mPEG, are more than 6-fold brighter in photoluminescence on the per mass basis, afford clear tumor imaging, and reach requisite photothermal tumor ablation temperatures with a >10-fold lower injected dose than as-synthesized SWCNT mixtures while exhibiting relatively low (6,5) accumulation in the reticuloendothelial system. The intravenous injection of ∼4 μg of (6,5) SWCNTs per mouse (0.254 mg/kg) for dual imaging/photothermal therapy is, by far, the lowest reported dose for nanoparticle-based in vivo therapeutics.

  View details for DOI 10.1021/nn4006472

  View details for Web of Science ID 000318143300081

  View details for PubMedID 23521224

• Strongly Coupled lnorganic/Nanocarbon Hybrid Materials for Advanced Electrocatalysis JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Liang, Y., Li, Y., Wang, H., Dai, H. 2013; 135 (6): 2013-2036

  Abstract

  Electrochemical systems, such as fuel cell and water splitting devices, represent some of the most efficient and environmentally friendly technologies for energy conversion and storage. Electrocatalysts play key roles in the chemical processes but often limit the performance of the entire systems due to insufficient activity, lifetime, or high cost. It has been a long-standing challenge to develop efficient and durable electrocatalysts at low cost. In this Perspective, we present our recent efforts in developing strongly coupled inorganic/nanocarbon hybrid materials to improve the electrocatalytic activities and stability of inorganic metal oxides, hydroxides, sulfides, and metal-nitrogen complexes. The hybrid materials are synthesized by direct nucleation, growth, and anchoring of inorganic nanomaterials on the functional groups of oxidized nanocarbon substrates including graphene and carbon nanotubes. This approach affords strong chemical attachment and electrical coupling between the electrocatalytic nanoparticles and nanocarbon, leading to nonprecious metal-based electrocatalysts with improved activity and durability for the oxygen reduction reaction for fuel cells and chlor-alkali catalysis, oxygen evolution reaction, and hydrogen evolution reaction. X-ray absorption near-edge structure and scanning transmission electron microscopy are employed to characterize the hybrids materials and reveal the coupling effects between inorganic nanomaterials and nanocarbon substrates. Z-contrast imaging and electron energy loss spectroscopy at single atom level are performed to investigate the nature of catalytic sites on ultrathin graphene sheets. Nanocarbon-based hybrid materials may present new opportunities for the development of electrocatalysts meeting the requirements of activity, durability, and cost for large-scale electrochemical applications.

  View details for DOI 10.1021/ja3089923

  View details for PubMedID 23339685

• Multiplexed cytokine detection on plasmonic gold substrates with enhanced near-infrared fluorescence NANO RESEARCH Zhang, B., Price, J., Hong, G., Tabakman, S. M., Wang, H., Jarrell, J. A., Feng, J., Utz, P. J., Dai, H. 2013; 6 (2): 113-120

  View details for DOI 10.1007/s12274-012-0286-2

  View details for Web of Science ID 000314763300004

• Single-Walled Carbon Nanotube Surface Control of Complement Recognition and Activation ACS NANO Andersen, A. J., Robinson, J. T., Dai, H., Hunter, A. C., Andresen, T. L., Moghimi, S. M. 2013; 7 (2): 1108-1119

  Abstract

  Carbon nanotubes (CNTs) are receiving considerable attention in site-specific drug and nucleic acid delivery, photodynamic therapy, and photoacoustic molecular imaging. Despite these advances, nanotubes may activate the complement system (an integral part of innate immunity), which can induce clinically significant anaphylaxis. We demonstrate that single-walled CNTs coated with human serum albumin activate the complement system through C1q-mediated classical and the alternative pathways. Surface coating with methoxypoly(ethylene glycol)-based amphiphiles, which confers solubility and prolongs circulation profiles of CNTs, activates the complement system differently, depending on the amphiphile structure. CNTs with linear poly(ethylene glycol) amphiphiles trigger the lectin pathway of the complement through both L-ficolin and mannan-binding lectin recognition. The lectin pathway activation, however, did not trigger the amplification loop of the alternative pathway. An amphiphile with branched poly(ethylene glycol) architecture also activated the lectin pathway but only through L-ficolin recognition. Importantly, this mode of activation neither generated anaphylatoxins nor induced triggering of the effector arm of the complement system. These observations provide a major step toward nanomaterial surface modification with polymers that have the properties to significantly improve innate immunocompatibility by limiting the formation of complement C3 and C5 convertases.

  View details for DOI 10.1021/nn3055175

  View details for Web of Science ID 000315618700027

  View details for PubMedID 23301860

• An integrated peptide-antigen microarray on plasmonic gold films for sensitive human antibody profiling. PloS one Zhang, B., Jarrell, J. A., Price, J. V., Tabakman, S. M., Li, Y., Gong, M., Hong, G., Feng, J., Utz, P. J., Dai, H. 2013; 8 (7)

  Abstract

  High-throughput screening for interactions of peptides with a variety of antibody targets could greatly facilitate proteomic analysis for epitope mapping, enzyme profiling, drug discovery and biomarker identification. Peptide microarrays are suited for such undertaking because of their high-throughput capability. However, existing peptide microarrays lack the sensitivity needed for detecting low abundance proteins or low affinity peptide-protein interactions. This work presents a new peptide microarray platform constructed on nanostructured plasmonic gold substrates capable of metal enhanced NIR fluorescence enhancement (NIR-FE) by hundreds of folds for screening peptide-antibody interactions with ultrahigh sensitivity. Further, an integrated histone peptide and whole antigen array is developed on the same plasmonic gold chip for profiling human antibodies in the sera of systemic lupus erythematosus (SLE) patients, revealing that collectively a panel of biomarkers against unmodified and post-translationally modified histone peptides and several whole antigens allow more accurate differentiation of SLE patients from healthy individuals than profiling biomarkers against peptides or whole antigens alone.

  View details for DOI 10.1371/journal.pone.0071043

  View details for PubMedID 23923050

• Advanced zinc-air batteries based on high-performance hybrid electrocatalysts. Nature communications Li, Y., Gong, M., Liang, Y., Feng, J., Kim, J., Wang, H., Hong, G., Zhang, B., Dai, H. 2013; 4: 1805-?

  Abstract

  Primary and rechargeable Zn-air batteries could be ideal energy storage devices with high energy and power density, high safety and economic viability. Active and durable electrocatalysts on the cathode side are required to catalyse oxygen reduction reaction during discharge and oxygen evolution reaction during charge for rechargeable batteries. Here we developed advanced primary and rechargeable Zn-air batteries with novel CoO/carbon nanotube hybrid oxygen reduction catalyst and Ni-Fe-layered double hydroxide oxygen evolution catalyst for the cathode. These catalysts exhibited higher catalytic activity and durability in concentrated alkaline electrolytes than precious metal Pt and Ir catalysts. The resulting primary Zn-air battery showed high discharge peak power density ~265 mW cm(-2), current density ~200 mA cm(-2) at 1 V and energy density >700 Wh kg(-1). Rechargeable Zn-air batteries in a tri-electrode configuration exhibited an unprecedented small charge-discharge voltage polarization of ~0.70 V at 20 mA cm(-2), high reversibility and stability over long charge and discharge cycles.

  View details for DOI 10.1038/ncomms2812

  View details for PubMedID 23651993

• Experimentally Engineering the Edge Termination of Graphene Nanoribbons ACS NANO Zhang, X., Yazyev, O. V., Feng, J., Xie, L., Tao, C., Chen, Y., Jiao, L., Pedramrazi, Z., Zettl, A., Louie, S. G., Dai, H., Crommie, M. F. 2013; 7 (1): 198-202

  Abstract

  The edges of graphene nanoribbons (GNRs) have attracted much interest due to their potentially strong influence on GNR electronic and magnetic properties. Here we report the ability to engineer the microscopic edge termination of high-quality GNRs via hydrogen plasma etching. Using a combination of high-resolution scanning tunneling microscopy and first-principles calculations, we have determined the exact atomic structure of plasma-etched GNR edges and established the chemical nature of terminating functional groups for zigzag, armchair, and chiral edge orientations. We find that the edges of hydrogen-plasma-etched GNRs are generally flat, free of structural reconstructions, and terminated by hydrogen atoms with no rehybridization of the outermost carbon edge atoms. Both zigzag and chiral edges show the presence of edge states.

  View details for DOI 10.1021/nn303730v

  View details for Web of Science ID 000314082800024

  View details for PubMedID 23194280

• Strongly coupled inorganic-nano-carbon hybrid materials for energy storage CHEMICAL SOCIETY REVIEWS Wang, H., Dai, H. 2013; 42 (7): 3088-3113

  Abstract

  The global shift of energy production from fossil fuels to renewable energy sources requires more efficient and reliable electrochemical energy storage devices. In particular, the development of electric or hydrogen powered vehicles calls for much-higher-performance batteries, supercapacitors and fuel cells than are currently available. In this review, we present an approach to synthesize electrochemical energy storage materials to form strongly coupled hybrids (SC-hybrids) of inorganic nanomaterials and novel graphitic nano-carbon materials such as carbon nanotubes and graphene, through nucleation and growth of nanoparticles at the functional groups of oxidized graphitic nano-carbon. We show that the inorganic-nano-carbon hybrid materials represent a new approach to synthesize electrode materials with higher electrochemical performance than traditional counterparts made by simple physical mixtures of electrochemically active inorganic particles and conducting carbon materials. The inorganic-nano-carbon hybrid materials are novel due to possible chemical bonding between inorganic nanoparticles and oxidized carbon, affording enhanced charge transport and increased rate capability of electrochemical materials without sacrificing specific capacity. Nano-carbon with various degrees of oxidation provides a novel substrate for nanoparticle nucleation and growth. The interactions between inorganic precursors and oxidized-carbon substrates provide a degree of control over the morphology, size and structure of the resulting inorganic nanoparticles. This paper reviews the recent development of inorganic-nano-carbon hybrid materials for electrochemical energy storage and conversion, including the preparation and functionalization of graphene sheets and carbon nanotubes to impart oxygen containing groups and defects, and methods of synthesis of nanoparticles of various morphologies on oxidized graphene and carbon nanotubes. We then review the applications of the SC-hybrid materials for high performance lithium ion batteries, rechargeable Li-S and Li-O2 batteries, supercapacitors and ultrafast Ni-Fe batteries, and new electrocatalysts for oxygen reduction, oxygen evolution and hydrogen evolution reactions.

  View details for DOI 10.1039/c2cs35307e

  View details for PubMedID 23361617

• Advanced zinc-air batteries based on high-performance hybrid electrocatalysts. Nature communications Li, Y., Gong, M., Liang, Y., Feng, J., Kim, J., Wang, H., Hong, G., Zhang, B., Dai, H. 2013; 4: 1805-?

  Abstract

  Primary and rechargeable Zn-air batteries could be ideal energy storage devices with high energy and power density, high safety and economic viability. Active and durable electrocatalysts on the cathode side are required to catalyse oxygen reduction reaction during discharge and oxygen evolution reaction during charge for rechargeable batteries. Here we developed advanced primary and rechargeable Zn-air batteries with novel CoO/carbon nanotube hybrid oxygen reduction catalyst and Ni-Fe-layered double hydroxide oxygen evolution catalyst for the cathode. These catalysts exhibited higher catalytic activity and durability in concentrated alkaline electrolytes than precious metal Pt and Ir catalysts. The resulting primary Zn-air battery showed high discharge peak power density ~265 mW cm(-2), current density ~200 mA cm(-2) at 1 V and energy density >700 Wh kg(-1). Rechargeable Zn-air batteries in a tri-electrode configuration exhibited an unprecedented small charge-discharge voltage polarization of ~0.70 V at 20 mA cm(-2), high reversibility and stability over long charge and discharge cycles.

  View details for DOI 10.1038/ncomms2812

  View details for PubMedID 23651993

• An integrated Peptide-antigen microarray on plasmonic gold films for sensitive human antibody profiling. PloS one Zhang, B., Jarrell, J. A., Price, J. V., Tabakman, S. M., Li, Y., Gong, M., Hong, G., Feng, J., Utz, P. J., Dai, H. 2013; 8 (7): e71043

  Abstract

  High-throughput screening for interactions of peptides with a variety of antibody targets could greatly facilitate proteomic analysis for epitope mapping, enzyme profiling, drug discovery and biomarker identification. Peptide microarrays are suited for such undertaking because of their high-throughput capability. However, existing peptide microarrays lack the sensitivity needed for detecting low abundance proteins or low affinity peptide-protein interactions. This work presents a new peptide microarray platform constructed on nanostructured plasmonic gold substrates capable of metal enhanced NIR fluorescence enhancement (NIR-FE) by hundreds of folds for screening peptide-antibody interactions with ultrahigh sensitivity. Further, an integrated histone peptide and whole antigen array is developed on the same plasmonic gold chip for profiling human antibodies in the sera of systemic lupus erythematosus (SLE) patients, revealing that collectively a panel of biomarkers against unmodified and post-translationally modified histone peptides and several whole antigens allow more accurate differentiation of SLE patients from healthy individuals than profiling biomarkers against peptides or whole antigens alone.

  View details for DOI 10.1371/journal.pone.0071043

  View details for PubMedID 23923050

  View details for PubMedCentralID PMC3726620

• Imaging state of charge and its correlation to interaction variation in an LiMn0.75Fe0.25PO4 nanorods-graphene hybrid CHEMICAL COMMUNICATIONS Zhou, J., Wang, J., Hu, Y., Regier, T., Wang, H., Yang, Y., Cui, Y., Dai, H. 2013; 49 (17): 1765-1767

  Abstract

  Visualization of the state of charge (SOC) in an LiMn(0.75)Fe(0.25)PO(4) nanorods-graphene hybrid nanostructure (LMFP-C) is realized by chemical mapping of the Fe valance state using scanning transmission X-ray microscopy (STXM). The LMFP-graphene interaction strength variation studied by C K-edge STXM has been correlated to SOC variation, i.e. a stronger interaction was observed for sample regions with a higher SOC in LMFP. Such structure-performance correlation opens new perspectives for a rational design of a better performance olivine cathode for lithium ion batteries.

  View details for DOI 10.1039/c3cc39015b

  View details for Web of Science ID 000314424700025

  View details for PubMedID 23340608

• Multifunctional in vivo vascular imaging using near-infrared II fluorescence NATURE MEDICINE Hong, G., Lee, J. C., Robinson, J. T., Raaz, U., Xie, L., Huang, N. F., Cooke, J. P., Dai, H. 2012; 18 (12): 1841-?

  Abstract

  In vivo real-time epifluorescence imaging of mouse hind limb vasculatures in the second near-infrared region (NIR-II) is performed using single-walled carbon nanotubes as fluorophores. Both high spatial (∼30 μm) and temporal (<200 ms per frame) resolution for small-vessel imaging are achieved at 1-3 mm deep in the hind limb owing to the beneficial NIR-II optical window that affords deep anatomical penetration and low scattering. This spatial resolution is unattainable by traditional NIR imaging (NIR-I) or microscopic computed tomography, and the temporal resolution far exceeds scanning microscopic imaging techniques. Arterial and venous vessels are unambiguously differentiated using a dynamic contrast-enhanced NIR-II imaging technique on the basis of their distinct hemodynamics. Further, the deep tissue penetration and high spatial and temporal resolution of NIR-II imaging allow for precise quantifications of blood velocity in both normal and ischemic femoral arteries, which are beyond the capabilities of ultrasonography at lower blood velocities.

  View details for DOI 10.1038/nm.2995

  View details for PubMedID 23160236

• Near infrared imaging and photothermal ablation of vascular inflammation using single-walled carbon nanotubes. Journal of the American Heart Association Kosuge, H., Sherlock, S. P., Kitagawa, T., Dash, R., Robinson, J. T., Dai, H., McConnell, M. V. 2012; 1 (6)

  Abstract

  Macrophages are critical contributors to atherosclerosis. Single-walled carbon nanotubes (SWNTs) show promising properties for cellular imaging and thermal therapy, which may have application to vascular macrophages.In vitro uptake and photothermal destruction of mouse macrophage cells (RAW264.7) were performed with SWNTs (14.7 nmol/L) exposed to an 808-nm light source. SWNTs were taken up by 94 ± 6% of macrophages, and light exposure induced 93 ± 3% cell death. In vivo vascular macrophage uptake and ablation were then investigated in carotid-ligated FVB mice (n=33) after induction of hyperlipidemia and diabetes. Two weeks postligation, near-infrared fluorescence (NIRF) carotid imaging (n=12) was performed with SWNT-Cy5.5 (8 nmol of Cy5.5) given via the tail vein. Photothermal heating and macrophage apoptosis were evaluated on freshly excised carotid arteries (n=21). NIRF of SWNTs showed higher signal intensity in ligated carotids compared with sham, confirmed by both in situ and ex vivo NIRF imaging (P<0.05, ligation versus sham). Immunofluorescence staining showed colocalization of SWNT-Cy5.5 and macrophages in atherosclerotic lesions. Light (808 nm) exposure of freshly excised carotids showed heating and induction of macrophage apoptosis in ligated left carotid arteries with SWNTs, but not in control groups without SWNTs or without light exposure.Carbon nanotubes accumulate in atherosclerotic macrophages in vivo and provide a multifunctional platform for imaging and photothermal therapy of vascular inflammation.

  View details for DOI 10.1161/JAHA.112.002568

  View details for PubMedID 23316318

• Chirality Enriched (12,1) and (11,3) Single-Walled Carbon Nanotubes for Biological Imaging JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Diao, S., Hong, G., Robinson, J. T., Jiao, L., Antaris, A. L., Wu, J. Z., Choi, C. L., Dai, H. 2012; 134 (41): 16971-16974

  Abstract

  The intrinsic band gap photoluminescence of semiconducting single-walled carbon nanotubes (SWNTs) makes them promising biological imaging probes in the second near-infrared (NIR-II, 1.0-1.4 μm) window. Thus far, SWNTs used for biological applications have been a complex mixture of metallic and semiconducting species with random chiralities, preventing simultaneous resonant excitation of all semiconducting nanotubes and emission at a single well-defined wavelength. Here, we developed a simple gel filtration method to enrich semiconducting (12,1) and (11,3) SWNTs with identical resonance absorption at ~808 nm and emission near ~1200 nm. The chirality sorted SWNTs showed ~5-fold higher photoluminescence intensity under resonant excitation of 808 nm than unsorted SWNTs on a per-mass basis. Real-time in vivo video imaging of whole mouse body and tumor vessels was achieved using a ~6-fold lower injected dose of (12,1) and (11,3) SWNTs (~3 μg per mouse or ~0.16 mg/kg of body weight vs 1.0 mg/kg for unsorted SWNTs) than a previous heterogeneous mixture, demonstrating the first resonantly excited and chirality separated SWNTs for biological imaging.

  View details for DOI 10.1021/ja307966u

  View details for Web of Science ID 000309854700014

  View details for PubMedID 23033937

• Engineering manganese oxide/nanocarbon hybrid materials for oxygen reduction electrocatalysis NANO RESEARCH Feng, J., Liang, Y., Wang, H., Li, Y., Zhang, B., Zhou, J., Wang, J., Regier, T., Dai, H. 2012; 5 (10): 718-725

  View details for DOI 10.1007/s12274-012-0256-8

  View details for Web of Science ID 000310087400006

• Oxygen Reduction Electrocatalyst Based on Strongly Coupled Cobalt Oxide Nanocrystals and Carbon Nanotubes JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Liang, Y., Wang, H., Diao, P., Chang, W., Hong, G., Li, Y., Gong, M., Xie, L., Zhou, J., Wang, J., Regier, T. Z., Wei, F., Dai, H. 2012; 134 (38): 15849-15857

  Abstract

  Electrocatalyst for oxygen reduction reaction (ORR) is crucial for a variety of renewable energy applications and energy-intensive industries. The design and synthesis of highly active ORR catalysts with strong durability at low cost is extremely desirable but remains challenging. Here, we used a simple two-step method to synthesize cobalt oxide/carbon nanotube (CNT) strongly coupled hybrid as efficient ORR catalyst by directly growing nanocrystals on oxidized multiwalled CNTs. The mildly oxidized CNTs provided functional groups on the outer walls to nucleate and anchor nanocrystals, while retaining intact inner walls for highly conducting network. Cobalt oxide was in the form of CoO due to a gas-phase annealing step in NH(3). The resulting CoO/nitrogen-doped CNT (NCNT) hybrid showed high ORR current density that outperformed Co(3)O(4)/graphene hybrid and commercial Pt/C catalyst at medium overpotential, mainly through a 4e reduction pathway. The metal oxide/carbon nanotube hybrid was found to be advantageous over the graphene counterpart in terms of active sites and charge transport. Last, the CoO/NCNT hybrid showed high ORR activity and stability under a highly corrosive condition of 10 M NaOH at 80 °C, demonstrating the potential of strongly coupled inorganic/nanocarbon hybrid as a novel catalyst system in oxygen depolarized cathode for chlor-alkali electrolysis.

  View details for DOI 10.1021/ja305623m

  View details for PubMedID 22957510

• Graphene hybrid nanomaterials for electrochemical energy storage and conversion Wang, H., Liang, Y., Li, Y., Yang, Y., Cui, Y., Dai, H. AMER CHEMICAL SOC. 2012

  View details for Web of Science ID 000324621804827

• Shape Matters: Intravital Microscopy Reveals Surprising Geometrical Dependence for Nanoparticles in Tumor Models of Extravasation NANO LETTERS Smith, B. R., Kempen, P., Bouley, D., Xu, A., Liu, Z., Melosh, N., Dai, H., Sinclair, R., Gambhir, S. S. 2012; 12 (7): 3369-3377

  Abstract

  Delivery is one of the most critical obstacles confronting nanoparticle use in cancer diagnosis and therapy. For most oncological applications, nanoparticles must extravasate in order to reach tumor cells and perform their designated task. However, little understanding exists regarding the effect of nanoparticle shape on extravasation. Herein we use real-time intravital microscopic imaging to meticulously examine how two different nanoparticles behave across three different murine tumor models. The study quantitatively demonstrates that high-aspect ratio single-walled carbon nanotubes (SWNTs) display extravasational behavior surprisingly different from, and counterintuitive to, spherical nanoparticles although the nanoparticles have similar surface coatings, area, and charge. This work quantitatively indicates that nanoscale extravasational competence is highly dependent on nanoparticle geometry and is heterogeneous.

  View details for DOI 10.1021/nl204175t

  View details for Web of Science ID 000306296200004

  View details for PubMedID 22650417

  View details for PubMedCentralID PMC3495189

• Rechargeable Li-O-2 batteries with a covalently coupled MnCo2O4-graphene hybrid as an oxygen cathode catalyst ENERGY & ENVIRONMENTAL SCIENCE Wang, H., Yang, Y., Liang, Y., Zheng, G., Li, Y., Cui, Y., Dai, H. 2012; 5 (7): 7931-7935

  View details for DOI 10.1039/c2ee21746e

  View details for Web of Science ID 000305530900032

• In Vivo Fluorescence Imaging in the Second Near-Infrared Window with Long Circulating Carbon Nanotubes Capable of Ultrahigh Tumor Uptake JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Robinson, J. T., Hong, G., Liang, Y., Zhang, B., Yaghi, O. K., Dai, H. 2012; 134 (25): 10664-10669

  Abstract

  Cancer imaging requires selective high accumulation of contrast agents in the tumor region and correspondingly low uptake in healthy tissues. Here, by making use of a novel synthetic polymer to solubilize single-walled carbon nanotubes (SWNTs), we prepared a well-functionalized SWNT formulation with long blood circulation (half-life of ∼30 h) in vivo to achieve ultrahigh accumulation of ∼30% injected dose (ID)/g in 4T1 murine breast tumors in Balb/c mice. Functionalization dependent blood circulation and tumor uptake were investigated through comparisons with phospholipid-PEG solubilized SWNTs. For the first time, we performed video-rate imaging of tumors based on the intrinsic fluorescence of SWNTs in the second near-infrared (NIR-II, 1.1-1.4 μm) window. We carried out dynamic contrast imaging through principal component analysis (PCA) to immediately pinpoint the tumor within ∼20 s after injection. Imaging over time revealed increasing tumor contrast up to 72 h after injection, allowing for its unambiguous identification. The 3D reconstruction of the SWNTs distribution based on their stable photoluminescence inside the tumor revealed a high degree of colocalization of SWNTs and blood vessels, suggesting enhanced permeability and retention (EPR) effect as the main cause of high passive tumor uptake of the nanotubes.

  View details for DOI 10.1021/ja303737a

  View details for Web of Science ID 000305716700052

  View details for PubMedID 22667448

  View details for PubMedCentralID PMC3471786

• Flexible Control of Block Copolymer Directed Self-Assembly using Small, Topographical Templates: Potential Lithography Solution for Integrated Circuit Contact Hole Patterning ADVANCED MATERIALS Yi, H., Bao, X., Zhang, J., Bencher, C., Chang, L., Chen, X., Tiberio, R., Conway, J., Dai, H., Chen, Y., Mitra, S., Wong, H. P. 2012; 24 (23): 3107-3114

  View details for DOI 10.1002/adma.201200265

  View details for Web of Science ID 000305121100015

  View details for PubMedID 22550028

• Family of Enhanced Photoacoustic Imaging Agents for High-Sensitivity and Multiplexing Studies in Living Mice ACS NANO de la Zerda, A., Bodapati, S., Teed, R., May, S. Y., Tabakman, S. M., Liu, Z., Khuri-Yakub, B. T., Chen, X., Dai, H., Gambhir, S. S. 2012; 6 (6): 4694-4701

  Abstract

  Photoacoustic imaging is a unique modality that overcomes to a great extent the resolution and depth limitations of optical imaging while maintaining relatively high contrast. However, since many diseases will not manifest an endogenous photoacoustic contrast, it is essential to develop exogenous photoacoustic contrast agents that can target diseased tissue(s). Here we present a family of novel photoacoustic contrast agents that are based on the binding of small optical dyes to single-walled carbon nanotubes (SWNT-dye). We synthesized five different SWNT-dye contrast agents using different optical dyes, creating five "flavors" of SWNT-dye nanoparticles. In particular, SWNTs that were coated with either QSY(21) (SWNT-QSY) or indocyanine green (SWNT-ICG) exhibited over 100-times higher photoacoustic contrast in living animals compared to plain SWNTs, leading to subnanomolar sensitivities. We then conjugated the SWNT-dye conjugates with cyclic Arg-Gly-Asp peptides to molecularly target the α(v)β(3) integrin, which is associated with tumor angiogenesis. Intravenous administration of these tumor-targeted imaging agents to tumor-bearing mice showed significantly higher photoacoustic signal in the tumor than in mice injected with the untargeted contrast agent. Finally, we were able to spectrally separate the photoacoustic signals of SWNT-QSY and SWNT-ICG in living animals injected subcutaneously with both particles in the same location, opening the possibility for multiplexing in vivo studies.

  View details for DOI 10.1021/nn204352r

  View details for Web of Science ID 000305661300017

  View details for PubMedID 22607191

  View details for PubMedCentralID PMC3397693

• An oxygen reduction electrocatalyst based on carbon nanotube-graphene complexes NATURE NANOTECHNOLOGY Li, Y., Zhou, W., Wang, H., Xie, L., Liang, Y., Wei, F., Idrobo, J., Pennycook, S. J., Dai, H. 2012; 7 (6): 394-400

  Abstract

  Oxygen reduction reaction catalysts based on precious metals such as platinum or its alloys are routinely used in fuel cells because of their high activity. Carbon-supported materials containing metals such as iron or cobalt as well as nitrogen impurities have been proposed to increase scalability and reduce costs, but these alternatives usually suffer from low activity and/or gradual deactivation during use. Here, we show that few-walled carbon nanotubes, following outer wall exfoliation via oxidation and high-temperature reaction with ammonia, can act as an oxygen reduction reaction electrocatalyst in both acidic and alkaline solutions. Under a unique oxidation condition, the outer walls of the few-walled carbon nanotubes are partially unzipped, creating nanoscale sheets of graphene attached to the inner tubes. The graphene sheets contain extremely small amounts of irons originated from nanotube growth seeds, and nitrogen impurities, which facilitate the formation of catalytic sites and boost the activity of the catalyst, as revealed by atomic-scale microscopy and electron energy loss spectroscopy. Whereas the graphene sheets formed from the unzipped part of the outer wall of the nanotubes are responsible for the catalytic activity, the inner walls remain intact and retain their electrical conductivity, which facilitates charge transport during electrocatalysis.

  View details for DOI 10.1038/NNANO.2012.72

  View details for PubMedID 22635099

• An ultrafast nickel-iron battery from strongly coupled inorganic nanoparticle/nanocarbon hybrid materials NATURE COMMUNICATIONS Wang, H., Liang, Y., Gong, M., Li, Y., Chang, W., Mefford, T., Zhou, J., Wang, J., Regier, T., Wei, F., Dai, H. 2012; 3

  Abstract

  Ultrafast rechargeable batteries made from low-cost and abundant electrode materials operating in safe aqueous electrolytes could be attractive for electrochemical energy storage. If both high specific power and energy are achieved, such batteries would be useful for power quality applications such as to assist propelling electric vehicles that require fast acceleration and intense braking. Here we develop a new type of Ni-Fe battery by employing novel inorganic nanoparticle/graphitic nanocarbon (carbon nanotubes and graphene) hybrid materials as electrode materials. We successfully increase the charging and discharging rates by nearly 1,000-fold over traditional Ni-Fe batteries while attaining high energy density. The ultrafast Ni-Fe battery can be charged in ~2 min and discharged within 30 s to deliver a specific energy of 120 Wh kg(-1) and a specific power of 15 kW kg(-1). These features suggest a new generation of Ni-Fe batteries as novel devices for electrochemical energy storage.

  View details for DOI 10.1038/ncomms1921

  View details for PubMedID 22735445

• Short channel field-effect transistors from highly enriched semiconducting carbon nanotubes NANO RESEARCH Wu, J., Xie, L., Hong, G., Lim, H. E., Thendie, B., Miyata, Y., Shinohara, H., Dai, H. 2012; 5 (6): 388-394

  View details for DOI 10.1007/s12274-012-0219-0

  View details for Web of Science ID 000305529900002

• Ag2S Quantum Dot: A Bright and Biocompatible Fluorescent Nanoprobe in the Second Near-Infrared Window ACS NANO Zhang, Y., Hong, G., Zhang, Y., Chen, G., Li, F., Dai, H., Wang, Q. 2012; 6 (5): 3695-3702

  Abstract

  Ag(2)S quantum dots (QDs) emitting in the second near-infrared region (NIR-II, 1.0-1.4 μm) are demonstrated as a promising fluorescent probe with both bright photoluminescence and high biocompatibility for the first time. Highly selective in vitro targeting and imaging of different cell lines are achieved using biocompatible NIR-II Ag(2)S QDs with different targeting ligands. The cytotoxicity study illustrates the Ag(2)S QDs with negligible effects in altering cell proliferation, triggering apoptosis and necrosis, generating reactive oxygen species, and causing DNA damage. Our results have opened up the possibilities of using these biocompatible Ag(2)S QDs for in vivo anatomical imaging and early stage tumor diagnosis with deep tissue penetration, high sensitivity, and elevated spatial and temporal resolution owing to their high emission efficiency in the unique NIR-II imaging window.

  View details for DOI 10.1021/nn301218z

  View details for Web of Science ID 000304231700007

  View details for PubMedID 22515909

  View details for PubMedCentralID PMC3358570

• In Operando X-ray Diffraction and Transmission X-ray Microscopy of Lithium Sulfur Batteries JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Nelson, J., Misra, S., Yang, Y., Jackson, A., Liu, Y., Wang, H., Dai, H., Andrews, J. C., Cui, Y., Toney, M. F. 2012; 134 (14): 6337-6343

  Abstract

  Rechargeable lithium-sulfur (Li-S) batteries hold great potential for high-performance energy storage systems because they have a high theoretical specific energy, low cost, and are eco-friendly. However, the structural and morphological changes during electrochemical reactions are still not well understood. In this Article, these changes in Li-S batteries are studied in operando by X-ray diffraction and transmission X-ray microscopy. We show recrystallization of sulfur by the end of the charge cycle is dependent on the preparation technique of the sulfur cathode. On the other hand, it was found that crystalline Li(2)S does not form at the end of discharge for all sulfur cathodes studied. Furthermore, during cycling the bulk of soluble polysulfides remains trapped within the cathode matrix. Our results differ from previous ex situ results. This highlights the importance of in operando studies and suggests possible strategies to improve cycle life.

  View details for DOI 10.1021/ja2121926

  View details for Web of Science ID 000302524800043

  View details for PubMedID 22432568

• Densely aligned graphene nanoribbons at similar to 35 nm pitch NANO RESEARCH Jiao, L., Xie, L., Dai, H. 2012; 5 (4): 292-296

  View details for DOI 10.1007/s12274-012-0209-2

  View details for Web of Science ID 000303408100008

• Covalent Hybrid of Spinel Manganese-Cobalt Oxide and Graphene as Advanced Oxygen Reduction Electrocatalysts JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Liang, Y., Wang, H., Zhou, J., Li, Y., Wang, J., Regier, T., Dai, H. 2012; 134 (7): 3517-3523

  Abstract

  Through direct nanoparticle nucleation and growth on nitrogen doped, reduced graphene oxide sheets and cation substitution of spinel Co(3)O(4) nanoparticles, a manganese-cobalt spinel MnCo(2)O(4)/graphene hybrid was developed as a highly efficient electrocatalyst for oxygen reduction reaction (ORR) in alkaline conditions. Electrochemical and X-ray near-edge structure (XANES) investigations revealed that the nucleation and growth method for forming inorganic-nanocarbon hybrids results in covalent coupling between spinel oxide nanoparticles and N-doped reduced graphene oxide (N-rmGO) sheets. Carbon K-edge and nitrogen K-edge XANES showed strongly perturbed C-O and C-N bonding in the N-rmGO sheet, suggesting the formation of C-O-metal and C-N-metal bonds between N-doped graphene oxide and spinel oxide nanoparticles. Co L-edge and Mn L-edge XANES suggested substitution of Co(3+) sites by Mn(3+), which increased the activity of the catalytic sites in the hybrid materials, further boosting the ORR activity compared with the pure cobalt oxide hybrid. The covalently bonded hybrid afforded much greater activity and durability than the physical mixture of nanoparticles and carbon materials including N-rmGO. At the same mass loading, the MnCo(2)O(4)/N-graphene hybrid can outperform Pt/C in ORR current density at medium overpotentials with stability superior to Pt/C in alkaline solutions.

  View details for DOI 10.1021/ja210924t

  View details for PubMedID 22280461

• Three-dimensional imaging of single nanotube molecule endocytosis on plasmonic substrates NATURE COMMUNICATIONS Hong, G., Wu, J. Z., Robinson, J. T., Wang, H., Zhang, B., Dai, H. 2012; 3

  Abstract

  Investigating the cellular internalization pathways of single molecules or single nano objects is important to understanding cell-matter interactions, and to applications in drug delivery and discovery. Imaging and tracking the motion of single molecules on cell plasma membranes require high spatial resolution in three dimensions. Fluorescence imaging along the axial dimension with nanometre resolution has been highly challenging, but critical to revealing displacements in transmembrane events. Here, utilizing a plasmonic ruler based on the sensitive distance dependence of near-infrared fluorescence enhancement of carbon nanotubes on a gold plasmonic substrate, we probe ~10 nm scale transmembrane displacements through changes in nanotube fluorescence intensity, enabling observations of single nanotube endocytosis in three dimensions. Cellular uptake and transmembrane displacements show clear dependences to temperature and clathrin assembly on cell membrane, suggesting that the cellular entry mechanism for a nanotube molecule is via clathrin-dependent endocytosis through the formation of clathrin-coated pits on the cell membrane.

  View details for DOI 10.1038/ncomms1698

  View details for PubMedID 22426221

• Graphite-Coated Magnetic Nanoparticle Microarray for Few-Cells Enrichment and Detection ACS NANO Chen, Z., Hong, G., Wang, H., Welsher, K., Tabakman, S. M., Sherlock, S. P., Robinson, J. T., Liang, Y., Dai, H. 2012; 6 (2): 1094-1101

  Abstract

  Graphite-coated, highly magnetic FeCo core-shell nanoparticles were synthesized by a chemical vapor deposition method and solubilized in aqueous solution through a unique polymer mixture modification, which significantly improved the biocompatibility and stability of the magnetic nanoparticles (MNPs). Such functionalized MNPs were proven to be very stable in different conditions which would be significant for biological applications. Cell staining, manipulation, enrichment, and detection were developed with these MNPs. Under external magnetic manipulation, the MNP-stained cells exhibited directed motions. Moreover, MNPs were printed on substrates to modulate the magnetic field distribution on the surface. Capture and detection of sparse populations of cancer cells spiked into whole blood has been explored in a microarray fashion. Cancer cells from hundreds down to only two were able to be simply and efficiently detected from 1 mL of whole blood on the MNP microarray chips. Interestingly, the cells captured through the MNP microarray still showed viability and adhered to the MNP spots after incubation, which could be utilized for cancer cell detection, localized growth, and proliferation.

  View details for DOI 10.1021/nn2034692

  View details for Web of Science ID 000300757900013

  View details for PubMedID 22229344

• Spectroscopic understanding of ultra-high rate performance for LiMn0.75Fe0.25PO4 nanorods-graphene hybrid in lithium ion battery PHYSICAL CHEMISTRY CHEMICAL PHYSICS Zhou, J., Wang, J., Zuin, L., Regier, T., Hu, Y., Wang, H., Liang, Y., Maley, J., Sammynaiken, R., Dai, H. 2012; 14 (27): 9578-9581

  Abstract

  Comprehensive X-ray absorption near-edge structure spectroscopy at the C, O and Li K-edges and the Mn, Fe, and P L-edges of LiMn(0.75)Fe(0.25)PO(4) nanorods-graphene has been reported in great detail. Compared to that of free standing graphene and LiMn(0.75)Fe(0.25)PO(4), the intimate interaction between the nanorods and graphene via charge redistribution has been unambiguously confirmed. This interaction not only anchors the nanorods onto the graphene but also modifies its surface chemistry, both of which afford the nanorods-graphene hybrid an ultra-high rate performance in lithium ion batteries. Such knowledge is important for the understanding of hybrid nanomaterials for lithium ion batteries and allows rational design for further improvements in performance.

  View details for DOI 10.1039/c2cp41012e

  View details for Web of Science ID 000305581500005

  View details for PubMedID 22678419

• In Vivo Fluorescence Imaging with Ag2S Quantum Dots in the Second Near-Infrared Region ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Hong, G., Robinson, J. T., Zhang, Y., Diao, S., Antaris, A. L., Wang, Q., Dai, H. 2012; 51 (39): 9818-9821

  Abstract

  Hits the dot: Ag(2)S quantum dots (QDs) with bright near-infrared-II fluorescence emission (around 1200 nm) and six-arm branched PEG surface coating were synthesized for in vivo small-animal imaging. The 6PEG-Ag(2)S QDs afforded a tumor uptake of approximately 10 % injected dose/gram, owing to a long circulation half-life of approximately 4 h. Clearance of the injected 6PEG-Ag(2)S QDs occurs mainly through the biliary pathway in mice.

  View details for DOI 10.1002/anie.201206059

  View details for Web of Science ID 000308886800018

  View details for PubMedID 22951900

• Controlled Chlorine Plasma Reaction for Noninvasive Graphene Doping JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Wu, J., Xie, L., Li, Y., Wang, H., Ouyang, Y., Guo, J., Dai, H. 2011; 133 (49): 19668-19671

  Abstract

  We investigated the chlorine plasma reaction with graphene and graphene nanoribbons and compared it with the hydrogen and fluorine plasma reactions. Unlike the rapid destruction of graphene by hydrogen and fluorine plasmas, much slower reaction kinetics between the chlorine plasma and graphene were observed, allowing for controlled chlorination. Electrical measurements on graphene sheets, graphene nanoribbons, and large graphene films grown by chemical vapor deposition showed p-type doping accompanied by a conductance increase, suggesting nondestructive doping via chlorination. Ab initio simulations were performed to rationalize the differences in fluorine, hydrogen, and chlorine functionalization of graphene.

  View details for DOI 10.1021/ja2091068

  View details for PubMedID 22082226

• Multifunctional FeCo-graphitic carbon nanocrystals for combined imaging, drug delivery and tumor-specific photothermal therapy in mice NANO RESEARCH Sherlock, S. P., Dai, H. 2011; 4 (12): 1248-1260

  View details for DOI 10.1007/s12274-011-0176-z

  View details for Web of Science ID 000297913800009

• Co3O4 nanocrystals on graphene as a synergistic catalyst for oxygen reduction reaction NATURE MATERIALS Liang, Y., Li, Y., Wang, H., Zhou, J., Wang, J., Regier, T., Dai, H. 2011; 10 (10): 780-786

  Abstract

  Catalysts for oxygen reduction and evolution reactions are at the heart of key renewable-energy technologies including fuel cells and water splitting. Despite tremendous efforts, developing oxygen electrode catalysts with high activity at low cost remains a great challenge. Here, we report a hybrid material consisting of Co₃O₄ nanocrystals grown on reduced graphene oxide as a high-performance bi-functional catalyst for the oxygen reduction reaction (ORR) and oxygen evolution reaction (OER). Although Co₃O₄ or graphene oxide alone has little catalytic activity, their hybrid exhibits an unexpected, surprisingly high ORR activity that is further enhanced by nitrogen doping of graphene. The Co₃O₄/N-doped graphene hybrid exhibits similar catalytic activity but superior stability to Pt in alkaline solutions. The same hybrid is also highly active for OER, making it a high-performance non-precious metal-based bi-catalyst for both ORR and OER. The unusual catalytic activity arises from synergetic chemical coupling effects between Co₃O₄ and graphene.

  View details for DOI 10.1038/NMAT3087

  View details for PubMedID 21822263

• Graphene nanoribbons with smooth edges behave as quantum wires NATURE NANOTECHNOLOGY Wang, X., Ouyang, Y., Jiao, L., Wang, H., Xie, L., Wu, J., Guo, J., Dai, H. 2011; 6 (9): 563-567

  Abstract

  Graphene nanoribbons with perfect edges are predicted to exhibit interesting electronic and spintronic properties, notably quantum-confined bandgaps and magnetic edge states. However, so far, graphene nanoribbons produced by lithography have had rough edges, as well as low-temperature transport characteristics dominated by defects (mainly variable range hopping between localized states in a transport gap near the Dirac point). Here, we report that one- and two-layer nanoribbon quantum dots made by unzipping carbon nanotubes exhibit well-defined quantum transport phenomena, including Coulomb blockade, the Kondo effect, clear excited states up to ∼20 meV, and inelastic co-tunnelling. Together with the signatures of intrinsic quantum-confined bandgaps and high conductivities, our data indicate that the nanoribbons behave as clean quantum wires at low temperatures, and are not dominated by defects.

  View details for DOI 10.1038/NNANO.2011.138

  View details for PubMedID 21873992

• Plasmonic substrates for multiplexed protein microarrays with femtomolar sensitivity and broad dynamic range NATURE COMMUNICATIONS Tabakman, S. M., Lau, L., Robinson, J. T., Price, J., Sherlock, S. P., Wang, H., Zhang, B., Chen, Z., Tangsombatvisit, S., Jarrell, J. A., Utz, P. J., Dai, H. 2011; 2

  Abstract

  Protein chips are widely used for high-throughput proteomic analysis, but to date, the low sensitivity and narrow dynamic range have limited their capabilities in diagnostics and proteomics. Here we present protein microarrays on a novel nanostructured, plasmonic gold film with near-infrared fluorescence enhancement of up to 100-fold, extending the dynamic range of protein detection by three orders of magnitude towards the fM regime. We employ plasmonic protein microarrays for the early detection of a cancer biomarker, carcinoembryonic antigen, in the sera of mice bearing a xenograft tumour model. Further, we demonstrate a multiplexed autoantigen array for human autoantibodies implicated in a range of autoimmune diseases with superior signal-to-noise ratios and broader dynamic range compared with commercial nitrocellulose and glass substrates. The high sensitivity, broad dynamic range and easy adaptability of plasmonic protein chips presents new opportunities in proteomic research and diagnostics applications.

  View details for DOI 10.1038/ncomms1477

  View details for PubMedID 21915108

• Advanced asymmetrical supercapacitors based on graphene hybrid materials NANO RESEARCH Wang, H., Liang, Y., Mirfakhrai, T., Chen, Z., Casalongue, H. S., Dai, H. 2011; 4 (8): 729-736

  View details for DOI 10.1007/s12274-011-0129-6

  View details for Web of Science ID 000293557500002

• Spatially resolving edge states of chiral graphene nanoribbons NATURE PHYSICS Tao, C., Jiao, L., Yazyev, O. V., Chen, Y., Feng, J., Zhang, X., Capaz, R. B., Tour, J. M., Zettl, A., Louie, S. G., Dai, H., Crommie, M. F. 2011; 7 (8): 616-620

  View details for DOI 10.1038/NPHYS1991

  View details for Web of Science ID 000293354000013

• Graphene Nanoribbons from Unzipped Carbon Nanotubes: Atomic Structures, Raman Spectroscopy, and Electrical Properties JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Xie, L., Wang, H., Jin, C., Wang, X., Jiao, L., Suenaga, K., Dai, H. 2011; 133 (27): 10394-10397

  Abstract

  We investigated the atomic structures, Raman spectroscopic and electrical transport properties of individual graphene nanoribbons (GNRs, widths ~10-30 nm) derived from sonochemical unzipping of multiwalled carbon nanotubes (MWNTs). Aberration-corrected transmission electron microscopy (TEM) revealed a high percentage of two-layer (2 L) GNRs and some single-layer ribbons. The layer-layer stacking angles ranged from 0° to 30° including average chiral angles near 30° (armchair orientation) or 0° (zigzag orientation). A large fraction of GNRs with bent and smooth edges was observed, while the rest showed flat and less smooth edges (roughness ≤1 nm). Polarized Raman spectroscopy probed individual GNRs to reveal D/G ratios and ratios of D band intensities at parallel and perpendicular laser excitation polarization (D(∥)/D(⊥)). The observed spectroscopic trends were used to infer the average chiral angles and edge smoothness of GNRs. Electrical transport and Raman measurements were carried out for individual ribbons to correlate spectroscopic and electrical properties of GNRs.

  View details for DOI 10.1021/ja203860a

  View details for PubMedID 21678963

• Graphene-Wrapped Sulfur Particles as a Rechargeable Lithium-Sulfur Battery Cathode Material with High Capacity and Cycling Stability NANO LETTERS Wang, H., Yang, Y., Liang, Y., Robinson, J. T., Li, Y., Jackson, A., Cui, Y., Dai, H. 2011; 11 (7): 2644-2647

  Abstract

  We report the synthesis of a graphene-sulfur composite material by wrapping poly(ethylene glycol) (PEG) coated submicrometer sulfur particles with mildly oxidized graphene oxide sheets decorated by carbon black nanoparticles. The PEG and graphene coating layers are important to accommodating volume expansion of the coated sulfur particles during discharge, trapping soluble polysulfide intermediates, and rendering the sulfur particles electrically conducting. The resulting graphene-sulfur composite showed high and stable specific capacities up to ∼600 mAh/g over more than 100 cycles, representing a promising cathode material for rechargeable lithium batteries with high energy density.

  View details for DOI 10.1021/nl200658a

  View details for PubMedID 21699259

• Carbon materials for drug delivery & cancer therapy MATERIALS TODAY Liu, Z., Robinson, J. T., Tabakman, S. M., Yang, K., Dai, H. 2011; 14 (7-8): 316-323

  View details for Web of Science ID 000292497100012

• Thermally Limited Current Carrying Ability of Graphene Nanoribbons PHYSICAL REVIEW LETTERS Liao, A. D., Wu, J. Z., Wang, X., Tahy, K., Jena, D., Dai, H., Pop, E. 2011; 106 (25)

  Abstract

  We investigate high-field transport in graphene nanoribbons (GNRs) on SiO(2), up to breakdown. The maximum current density is limited by self-heating, but can reach >3 mA/μm for GNRs ~15 nm wide. Comparison with larger, micron-sized graphene devices reveals that narrow GNRs benefit from 3D heat spreading into the SiO(2), which enables their higher current density. GNRs also benefit from lateral heat flow to the contacts in short devices (<~0.3 μm), which allows extraction of a median GNR thermal conductivity (TC), ~80 W m(-1)K(-1) at 20 °C across our samples, dominated by phonons. The TC of GNRs is an order of magnitude lower than that of micron-sized graphene on SiO(2), suggesting strong roles of edge and defect scattering, and the importance of thermal dissipation in small GNR devices.

  View details for DOI 10.1103/PhysRevLett.106.256801

  View details for Web of Science ID 000291801900010

  View details for PubMedID 21770659

• Deep-tissue anatomical imaging of mice using carbon nanotube fluorophores in the second near-infrared window PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Welsher, K., Sherlock, S. P., Dai, H. 2011; 108 (22): 8943-8948

  Abstract

  Fluorescent imaging in the second near-infrared window (NIR II, 1-1.4 μm) holds much promise due to minimal autofluorescence and tissue scattering. Here, using well-functionalized biocompatible single-walled carbon nanotubes (SWNTs) as NIR II fluorescent imaging agents, we performed high-frame-rate video imaging of mice during intravenous injection of SWNTs and investigated the path of SWNTs through the mouse anatomy. We observed in real-time SWNT circulation through the lungs and kidneys several seconds postinjection, and spleen and liver at slightly later time points. Dynamic contrast-enhanced imaging through principal component analysis (PCA) was performed and found to greatly increase the anatomical resolution of organs as a function of time postinjection. Importantly, PCA was able to discriminate organs such as the pancreas, which could not be resolved from real-time raw images. Tissue phantom studies were performed to compare imaging in the NIR II region to the traditional NIR I biological transparency window (700-900 nm). Examination of the feature sizes of a common NIR I dye (indocyanine green) showed a more rapid loss of feature contrast and integrity with increasing feature depth as compared to SWNTs in the NIR II region. The effects of increased scattering in the NIR I versus NIR II region were confirmed by Monte Carlo simulation. In vivo fluorescence imaging in the NIR II region combined with PCA analysis may represent a powerful approach to high-resolution optical imaging through deep tissues, useful for a wide range of applications from biomedical research to disease diagnostics.

  View details for DOI 10.1073/pnas.1014501108

  View details for Web of Science ID 000291106200015

  View details for PubMedID 21576494

  View details for PubMedCentralID PMC3107273

• MoS2 Nanoparticles Grown on Graphene: An Advanced Catalyst for the Hydrogen Evolution Reaction JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Li, Y., Wang, H., Xie, L., Liang, Y., Hong, G., Dai, H. 2011; 133 (19): 7296-7299

  Abstract

  Advanced materials for electrocatalytic and photoelectrochemical water splitting are central to the area of renewable energy. In this work, we developed a selective solvothermal synthesis of MoS(2) nanoparticles on reduced graphene oxide (RGO) sheets suspended in solution. The resulting MoS(2)/RGO hybrid material possessed nanoscopic few-layer MoS(2) structures with an abundance of exposed edges stacked onto graphene, in strong contrast to large aggregated MoS(2) particles grown freely in solution without GO. The MoS(2)/RGO hybrid exhibited superior electrocatalytic activity in the hydrogen evolution reaction (HER) relative to other MoS(2) catalysts. A Tafel slope of ∼41 mV/decade was measured for MoS(2) catalysts in the HER for the first time; this exceeds by far the activity of previous MoS(2) catalysts and results from the abundance of catalytic edge sites on the MoS(2) nanoparticles and the excellent electrical coupling to the underlying graphene network. The ∼41 mV/decade Tafel slope suggested the Volmer-Heyrovsky mechanism for the MoS(2)-catalyzed HER, with electrochemical desorption of hydrogen as the rate-limiting step.

  View details for DOI 10.1021/ja201269b

  View details for PubMedID 21510646

• Ultrasmall Reduced Graphene Oxide with High Near-Infrared Absorbance for Photothermal Therapy JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Robinson, J. T., Tabakman, S. M., Liang, Y., Wang, H., Casalongue, H. S., Daniel Vinh, D., Dai, H. 2011; 133 (17): 6825-6831

  Abstract

  We developed nanosized, reduced graphene oxide (nano-rGO) sheets with high near-infrared (NIR) light absorbance and biocompatibility for potential photothermal therapy. The single-layered nano-rGO sheets were ∼20 nm in average lateral dimension, functionalized noncovalently by amphiphilic PEGylated polymer chains to render stability in biological solutions and exhibited 6-fold higher NIR absorption than nonreduced, covalently PEGylated nano-GO. Attaching a targeting peptide bearing the Arg-Gly-Asp (RGD) motif to nano-rGO afforded selective cellular uptake in U87MG cancer cells and highly effective photoablation of cells in vitro. In the absence of any NIR irradiation, nano-rGO exhibited little toxicity in vitro at concentrations well above the doses needed for photothermal heating. This work established nano-rGO as a novel photothermal agent due to its small size, high photothermal efficiency, and low cost as compared to other NIR photothermal agents including gold nanomaterials and carbon nanotubes.

  View details for DOI 10.1021/ja2010175

  View details for PubMedID 21476500

• Hydrogen Spillover in Pt-Single-Walled Carbon Nanotube Composites: Formation of Stable C-H Bonds JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Bhowmick, R., Rajasekaran, S., Friebel, D., Beasley, C., Jiao, L., Ogasawara, H., Dai, H., Clemens, B., Nilsson, A. 2011; 133 (14): 5580-5586

  Abstract

  Using in situ electrical conductivity and ex situ X-ray photoelectron spectroscopy (XPS) measurements, we have examined how the hydrogen uptake of single-walled carbon nanotubes (SWNTs) is influenced by the addition of Pt nanoparticles. The conductivity of platinum-sputtered single-walled carbon nanotubes (Pt-SWNTs) during molecular hydrogen exposure decreased more rapidly than that of the corresponding pure SWNTs, which supports a hydrogenation mechanism facilitated by "spillover" of dissociated hydrogen from the Pt nanoparticles. C 1s XPS spectra indicate that the Pt-SWNTs store hydrogen by means of chemisorption, that is, covalent C-H bond formation: molecular hydrogen charging at elevated pressure (8.27 bar) and room temperature yielded Pt-SWNTs with up to 16 ± 1.5 at. % sp(3)-hybridized carbon atoms, which corresponds to a hydrogen-storage capacity of 1.2 wt % (excluding the weight of Pt nanoparticles). Pt-SWNTs prepared by the Langmuir-Blodgett (LB) technique exhibited the highest Pt/SWNT ratio and also the best hydrogen uptake.

  View details for DOI 10.1021/ja200403m

  View details for Web of Science ID 000289829100060

  View details for PubMedID 21428292

• Solution-phase growth of plasmonic gold films for surface-enhanced Raman scattering and metal-enhanced fluorescence detection applications 241st National Meeting and Exposition of the American-Chemical-Society (ACS) Tabakman, S. M., Chen, Z., Wang, H., Robinson, J. T., Dai, H. AMER CHEMICAL SOC. 2011

  View details for Web of Science ID 000291982801436

• FeCo-Graphitic carbon nanocrystals as multifunctional imaging and therapeutic agents 241st National Meeting and Exposition of the American-Chemical-Society (ACS) Sherlock, S. P., Tabakman, S. M., Dai, H. AMER CHEMICAL SOC. 2011

  View details for Web of Science ID 000291982803628

• Graphene-based hybrid nanomaterials for energy storage applications 241st National Meeting and Exposition of the American-Chemical-Society (ACS) Wang, H., Liang, Y., Sanchez, H., Yang, Y., Cui, L., Cui, Y., Dai, H. AMER CHEMICAL SOC. 2011

  View details for Web of Science ID 000291982803672

• Room-Temperature Edge Functionalization and Doping of Graphene by Mild Plasma SMALL Kato, T., Jiao, L., Wang, X., Wang, H., Li, X., Zhang, L., Hatakeyama, R., Dai, H. 2011; 7 (5): 574-577

  View details for DOI 10.1002/smll.201002146

  View details for Web of Science ID 000288081900004

  View details for PubMedID 21370457

• A New Approach to Solution-Phase Gold Seeding for SERS Substrates SMALL Tabakman, S. M., Chen, Z., Casalongue, H. S., Wang, H., Dai, H. 2011; 7 (4): 499-505

  Abstract

  Surface-enhanced Raman scattering (SERS) vastly improves signal-to-noise ratios as compared to traditional Raman scattering, making sensitive assays based upon Raman scattering a reality. However, preparation of highly stable SERS-active gold substrates requires complicated and expensive methodologies and instrumentation. Here, a general and completely solution-phase, seed-based approach is introduced, which is capable of producing gold films for SERS applications on a variety of substrates, not requiring surface modification or functionalization. SERS enhancement factors of ≈10(7) were observed. Moreover, solution-phase gold film deposition on highly complex surfaces, such as protein-coated bioassays, is demonstrated for the first time. Protein bioassays coated with such SERS-active gold films are combined with bioconjugated single-walled carbon nanotube Raman labels, affording highly sensitive detection of the cancer biomarker, carcinoembryonic antigen in serum, with a limit of detection of ≈5 fM (1 pg mL(-1) ).

  View details for DOI 10.1002/smll.201001836

  View details for PubMedID 21360809

• Photothermally Enhanced Drug Delivery by Ultrasmall Multifunctional FeCo/Graphitic Shell Nanocrystals ACS NANO Sherlock, S. P., Tabakman, S. M., Xie, L., Dai, H. 2011; 5 (2): 1505-1512

  Abstract

  FeCo/graphitic carbon shell (FeCo/GC) nanocrystals (∼4-5 nm in diameter) with ultrahigh magnetization are synthesized, functionalized, and developed into multifunctional biocompatible materials. We demonstrate the ability of this material to serve as an integrated system for combined drug delivery, near-infrared (NIR) photothermal therapy, and magnetic resonance imaging (MRI) in vitro. We show highly efficient loading of doxorubicin (DOX) by π-stacking on the graphitic shell to afford FeCo/GC-DOX complexes and pH sensitive DOX release from the particles. We observe enhanced intracellular drug delivery by FeCo/GC-DOX under 20 min of NIR laser (808 nm) induced hyperthermia to 43 °C, resulting in a significant increase of FeCo/GC-DOX toxicity toward breast cancer cells. The synergistic cancer cell killing by FeCo/GC-DOX drug delivery under photothermal heating is due to a ∼two-fold enhancement of cancer cell uptake of FeCo/GC-DOX complex and the increased DOX toxicity under the 43 °C hyperthermic condition. The combination of synergistic NIR photothermally enhanced drug delivery and MRI with the FeCo/GC nanocrystals could lead to a powerful multimodal system for biomedical detection and therapy.

  View details for DOI 10.1021/nn103415x

  View details for Web of Science ID 000287553800094

  View details for PubMedID 21284398

  View details for PubMedCentralID PMC3043169

• FeCo/Graphite Nanocrystals for Multi-Modality Imaging of Experimental Vascular Inflammation PLOS ONE Kosuge, H., Sherlock, S. P., Kitagawa, T., Terashima, M., Barral, J. K., Nishimura, D. G., Dai, H., McConnell, M. V. 2011; 6 (1)

  Abstract

  FeCo/graphitic-carbon nanocrystals (FeCo/GC) are biocompatible, high-relaxivity, multi-functional nanoparticles. Macrophages represent important cellular imaging targets for assessing vascular inflammation. We evaluated FeCo/GC for vascular macrophage uptake and imaging in vivo using fluorescence and MRI.Hyperlipidemic and diabetic mice underwent carotid ligation to produce a macrophage-rich vascular lesion. In situ and ex vivo fluorescence imaging were performed at 48 hours after intravenous injection of FeCo/GC conjugated to Cy5.5 (n = 8, 8 nmol of Cy5.5/mouse). Significant fluorescence signal from FeCo/GC-Cy5.5 was present in the ligated left carotid arteries, but not in the control (non-ligated) right carotid arteries or sham-operated carotid arteries (p = 0.03 for ligated vs. non-ligated). Serial in vivo 3T MRI was performed at 48 and 72 hours after intravenous FeCo/GC (n = 6, 270 µg Fe/mouse). Significant T2* signal loss from FeCo/GC was seen in ligated left carotid arteries, not in non-ligated controls (p = 0.03). Immunofluorescence staining showed colocalization of FeCo/GC and macrophages in ligated carotid arteries.FeCo/GC accumulates in vascular macrophages in vivo, allowing fluorescence and MR imaging. This multi-functional high-relaxivity nanoparticle platform provides a promising approach for cellular imaging of vascular inflammation.

  View details for DOI 10.1371/journal.pone.0014523

  View details for PubMedID 21264237

• LiMn1-xFexPO4 Nanorods Grown on Graphene Sheets for Ultrahigh-Rate-Performance Lithium Ion Batteries ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Wang, H., Yang, Y., Liang, Y., Cui, L., Casalongue, H. S., Li, Y., Hong, G., Cui, Y., Dai, H. 2011; 50 (32): 7364-7368

  View details for DOI 10.1002/anie.201103163

  View details for PubMedID 21710671

• Near-Infrared-Fluorescence-Enhanced Molecular Imaging of Live Cells on Gold Substrates ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Hong, G., Tabakman, S. M., Welsher, K., Chen, Z., Robinson, J. T., Wang, H., Zhang, B., Dai, H. 2011; 50 (20): 4644-4648

  View details for DOI 10.1002/anie.201100934

  View details for PubMedID 21506225

• Co1-xS-Graphene Hybrid: A High-Performance Metal Chalcogenide Electrocatalyst for Oxygen Reduction ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Wang, H., Liang, Y., Li, Y., Dai, H. 2011; 50 (46): 10969-10972

  View details for DOI 10.1002/anie.201104004

  View details for PubMedID 21954126

• A Dual Platform for Selective Analyte Enrichment and Ionization in Mass Spectrometry Using Aptamer-Conjugated Graphene Oxide JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Gulbakan, B., Yasun, E., Shukoor, M. I., Zhu, Z., You, M., Tan, X., Sanchez, H., Powell, D. H., Dai, H., Tan, W. 2010; 132 (49): 17408-17410

  Abstract

  This study demonstrates the use of aptamer-conjugated graphene oxide as an affinity extraction and detection platform for analytes from complex biological media. We have shown that cocaine and adenosine can be selectively enriched from plasma samples and that direct mass spectrometric readouts can be obtained without a matrix and with greatly improved signal-to-noise ratios. Aptamer-conjugated graphene oxide has clear advantages in target enrichment and in generating highly efficient ionization of target molecules for mass spectrometry. These results demonstrate the utility of the approach for analysis of small molecules in real biological samples.

  View details for DOI 10.1021/ja109042w

  View details for Web of Science ID 000285328800024

  View details for PubMedID 21090719

  View details for PubMedCentralID PMC3135746

• Optical Properties of Single-Walled Carbon Nanotubes Separated in a Density Gradient: Length, Bundling, and Aromatic Stacking Effects JOURNAL OF PHYSICAL CHEMISTRY C Tabakman, S. M., Welsher, K., Hong, G., Dai, H. 2010; 114 (46): 19569-19575

  Abstract

  Single-walled carbon nanotubes (SWNTs) are promising materials for in vitro and in vivo biological applications due to their high surface area and inherent near infrared photoluminescence and Raman scattering properties. Here, we use density gradient centrifugation to separate SWNTs by length and degree of bundling. Following separation, we observe a peak in photoluminescence quantum yield (PL QY) and Raman scattering intensity where SWNT length is maximized and bundling is minimized. Individualized SWNTs are found to exhibit high PL QY and high resonance-enhanced Raman scattering intensity. Fractions containing long, individual SWNTs exhibit the highest PL QY and Raman scattering intensities, compared to fractions containing single, short SWNTs or SWNT bundles. Intensity gains of approximately ~1.7 and 4-fold, respectively, are obtained compared with the starting material. Spectroscopic analysis reveals that SWNT fractions at higher displacement contain increasing proportions of SWNT bundles, which causes reduced optical transition energies and broadening of absorption features in the UV-Vis-NIR spectra, and reduced PL QY and Raman scattering intensity. Finally, we adsorb small aromatic species on "bright," individualized SWNT sidewalls and compare the resulting absorption, PL and Raman scattering effects to that of SWNT bundles. We observe similar effects in both cases, suggesting aromatic stacking affects the optical properties of SWNTs in an analogous way to SWNT bundles, likely due to electronic structure perturbations, charge transfer, and dielectric screening effects, resulting in reduction of the excitonic optical transition energies and exciton lifetimes.

  View details for DOI 10.1021/jp106453v

  View details for Web of Science ID 000284287900003

  View details for PubMedCentralID PMC3023917

• Metal-Enhanced Fluorescence of Carbon Nanotubes JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Hong, G., Tabakman, S. M., Welsher, K., Wang, H., Wang, X., Dai, H. 2010; 132 (45): 15920-15923

  Abstract

  The photoluminescence (PL) quantum yield of single-walled carbon nanotubes (SWNTs) is relatively low, with various quenching effects by metallic species reported in the literature. Here, we report the first case of metal enhanced fluorescence (MEF) of surfactant-coated carbon nanotubes on nanostructured gold substrates. The photoluminescence quantum yield of SWNTs is observed to be enhanced more than 10-fold. The dependence of fluorescence enhancement on metal-nanotube distance and on the surface plasmon resonance (SPR) of the gold substrate for various SWNT chiralities is measured to reveal the mechanism of enhancement. Surfactant-coated SWNTs in direct contact with metal exhibit strong MEF without quenching, suggesting a small quenching distance for SWNTs on the order of the van der Waals distance, beyond which the intrinsically fast nonradiative decay rate in nanotubes is little enhanced by metal. The metal enhanced fluorescence of SWNTs is attributed to radiative lifetime shortening through resonance coupling of SWNT emission to the reradiating dipolar plasmonic modes in the metal.

  View details for DOI 10.1021/ja1087997

  View details for PubMedID 20979398

• High Performance In Vivo Near-IR (> 1 mu m) Imaging and Photothermal Cancer Therapy with Carbon Nanotubes NANO RESEARCH Robinson, J. T., Welsher, K., Tabakman, S. M., Sherlock, S. P., Wang, H., Luong, R., Dai, H. 2010; 3 (11): 779-793

  Abstract

  Short single-walled carbon nanotubes (SWNTs) functionalized by PEGylated phospholipids are biologically non-toxic and long-circulating nanomaterials with intrinsic near infrared photoluminescence (NIR PL), characteristic Raman spectra, and strong optical absorbance in the near infrared (NIR). This work demonstrates the first dual application of intravenously injected SWNTs as photoluminescent agents for in vivo tumor imaging in the 1.0-1.4 μm emission region and as NIR absorbers and heaters at 808 nm for photothermal tumor elimination at the lowest injected dose (70 μg of SWNT/mouse, equivalent to 3.6 mg/kg) and laser irradiation power (0.6 W/cm(2)) reported to date. Ex vivo resonance Raman imaging revealed the SWNT distribution within tumors at a high spatial resolution. Complete tumor elimination was achieved for large numbers of photothermally treated mice without any toxic side effects after more than six months post-treatment. Further, side-by-side experiments were carried out to compare the performance of SWNTs and gold nanorods (AuNRs) at an injected dose of 700 μg of AuNR/mouse (equivalent to 35 mg/kg) in NIR photothermal ablation of tumors in vivo. Highly effective tumor elimination with SWNTs was achieved at 10 times lower injected doses and lower irradiation powers than for AuNRs. These results suggest there are significant benefits of utilizing the intrinsic properties of biocompatible SWNTs for combined cancer imaging and therapy.

  View details for DOI 10.1007/s12274-010-0045-1

  View details for Web of Science ID 000284158700003

  View details for PubMedCentralID PMC3143483

• Carbon Nanotubes Enable Noninvasive Optical Imaging of Macrophages in Mouse Atherosclerosis and Have Intrinsic Fluorescence for Near Infrared Imaging Scientific Sessions on Arteriosclerosis, Thrombosis and Vascular Biology Kitagawa, T., Kosuge, H., Sherlock, S., Bogyo, M., Dai, H., McConnell, M. LIPPINCOTT WILLIAMS & WILKINS. 2010: E298–E298

  View details for Web of Science ID 000283234800519

• Optical Properties of Single-Walled Carbon Nanotubes Separated in a Density Gradient; Length, Bundling, and Aromatic Stacking Effects. The journal of physical chemistry. C, Nanomaterials and interfaces Tabakman, S. M., Welsher, K., Hong, G., Dai, H. 2010; 114 (46): 19569-19575

  Abstract

  Single-walled carbon nanotubes (SWNTs) are promising materials for in vitro and in vivo biological applications due to their high surface area and inherent near infrared photoluminescence and Raman scattering properties. Here, we use density gradient centrifugation to separate SWNTs by length and degree of bundling. Following separation, we observe a peak in photoluminescence quantum yield (PL QY) and Raman scattering intensity where SWNT length is maximized and bundling is minimized. Individualized SWNTs are found to exhibit high PL QY and high resonance-enhanced Raman scattering intensity. Fractions containing long, individual SWNTs exhibit the highest PL QY and Raman scattering intensities, compared to fractions containing single, short SWNTs or SWNT bundles. Intensity gains of approximately ~1.7 and 4-fold, respectively, are obtained compared with the starting material. Spectroscopic analysis reveals that SWNT fractions at higher displacement contain increasing proportions of SWNT bundles, which causes reduced optical transition energies and broadening of absorption features in the UV-Vis-NIR spectra, and reduced PL QY and Raman scattering intensity. Finally, we adsorb small aromatic species on "bright," individualized SWNT sidewalls and compare the resulting absorption, PL and Raman scattering effects to that of SWNT bundles. We observe similar effects in both cases, suggesting aromatic stacking affects the optical properties of SWNTs in an analogous way to SWNT bundles, likely due to electronic structure perturbations, charge transfer, and dielectric screening effects, resulting in reduction of the excitonic optical transition energies and exciton lifetimes.

  View details for DOI 10.1021/jp106453v

  View details for PubMedID 21258607

  View details for PubMedCentralID PMC3023917

• Selective Etching of Graphene Edges by Hydrogen Plasma JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Xie, L., Jiao, L., Dai, H. 2010; 132 (42): 14751-14753

  Abstract

  We devised a controlled hydrogen plasma reaction at 300 °C to etch graphene and graphene nanoribbons (GNRs) selectively at the edges over the basal plane. Atomic force microscope imaging showed that the etching rates for single-layer and few-layer (≥2 layers) graphene are 0.27 ± 0.05 nm/min and 0.10 ± 0.03 nm/min, respectively. Meanwhile, Raman spectroscopic mapping revealed no D band in the planes of single-layer or few-layer graphene after the plasma reaction, suggesting selective etching at the graphene edges without introducing defects in the basal plane. We found that hydrogen plasma at lower temperature (room temperature) or a higher temperature (500 °C) could hydrogenate the basal plane or introduce defects in the basal plane. Using the hydrogen plasma reaction at the intermediate temperature (300 °C), we obtained narrow, presumably hydrogen terminated GNRs (sub-5 nm) by etching of wide GNRs derived from unzipping of multiwalled carbon nanotubes. Such GNRs exhibited semiconducting characteristics with high on/off ratios (∼1000) in GNR field effect transistor devices at room temperature.

  View details for DOI 10.1021/ja107071g

  View details for Web of Science ID 000283403200021

  View details for PubMedID 20923144

• Mn3O4-Graphene Hybrid as a High-Capacity Anode Material for Lithium Ion Batteries JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Wang, H., Cui, L., Yang, Y., Casalongue, H. S., Robinson, J. T., Liang, Y., Cui, Y., Dai, H. 2010; 132 (40): 13978-13980

  Abstract

  We developed two-step solution-phase reactions to form hybrid materials of Mn(3)O(4) nanoparticles on reduced graphene oxide (RGO) sheets for lithium ion battery applications. Selective growth of Mn(3)O(4) nanoparticles on RGO sheets, in contrast to free particle growth in solution, allowed for the electrically insulating Mn(3)O(4) nanoparticles to be wired up to a current collector through the underlying conducting graphene network. The Mn(3)O(4) nanoparticles formed on RGO show a high specific capacity up to ∼900 mAh/g, near their theoretical capacity, with good rate capability and cycling stability, owing to the intimate interactions between the graphene substrates and the Mn(3)O(4) nanoparticles grown atop. The Mn(3)O(4)/RGO hybrid could be a promising candidate material for a high-capacity, low-cost, and environmentally friendly anode for lithium ion batteries. Our growth-on-graphene approach should offer a new technique for the design and synthesis of battery electrodes based on highly insulating materials.

  View details for DOI 10.1021/ja105296a

  View details for PubMedID 20853844

• TiO2 Nanocrystals Grown on Graphene as Advanced Photocatalytic Hybrid Materials NANO RESEARCH Liang, Y., Wang, H., Casalongue, H. S., Chen, Z., Dai, H. 2010; 3 (10): 701-705

  View details for DOI 10.1007/s12274-010-0033-5

  View details for Web of Science ID 000284017100003

• High Performance In Vivo Near-IR (>1 μm) Imaging and Photothermal Cancer Therapy with Carbon Nanotubes. Nano research Robinson, J. T., Welsher, K., Tabakman, S. M., Sherlock, S. P., Wang, H., Luong, R., Dai, H. 2010; 3 (11): 779-793

  Abstract

  Short single-walled carbon nanotubes (SWNTs) functionalized by PEGylated phospholipids are biologically non-toxic and long-circulating nanomaterials with intrinsic near infrared photoluminescence (NIR PL), characteristic Raman spectra, and strong optical absorbance in the near infrared (NIR). This work demonstrates the first dual application of intravenously injected SWNTs as photoluminescent agents for in vivo tumor imaging in the 1.0-1.4 μm emission region and as NIR absorbers and heaters at 808 nm for photothermal tumor elimination at the lowest injected dose (70 μg of SWNT/mouse, equivalent to 3.6 mg/kg) and laser irradiation power (0.6 W/cm(2)) reported to date. Ex vivo resonance Raman imaging revealed the SWNT distribution within tumors at a high spatial resolution. Complete tumor elimination was achieved for large numbers of photothermally treated mice without any toxic side effects after more than six months post-treatment. Further, side-by-side experiments were carried out to compare the performance of SWNTs and gold nanorods (AuNRs) at an injected dose of 700 μg of AuNR/mouse (equivalent to 35 mg/kg) in NIR photothermal ablation of tumors in vivo. Highly effective tumor elimination with SWNTs was achieved at 10 times lower injected doses and lower irradiation powers than for AuNRs. These results suggest there are significant benefits of utilizing the intrinsic properties of biocompatible SWNTs for combined cancer imaging and therapy.

  View details for DOI 10.1007/s12274-010-0045-1

  View details for PubMedID 21804931

  View details for PubMedCentralID PMC3143483

• Etching and narrowing of graphene from the edges NATURE CHEMISTRY Wang, X., Dai, H. 2010; 2 (8): 661-665

  Abstract

  Large-scale graphene electronics requires lithographic patterning of narrow graphene nanoribbons for device integration. However, conventional lithography can only reliably pattern approximately 20-nm-wide GNR arrays limited by lithography resolution, while sub-5-nm GNRs are desirable for high on/off ratio field-effect transistors at room temperature. Here, we devised a gas phase chemical approach to etch graphene from the edges without damaging its basal plane. The reaction involved high temperature oxidation of graphene in a slightly reducing environment in the presence of ammonia to afford controlled etch rate (less than or approximately 1 nm min(-1)). We fabricated approximately 20-30-nm-wide graphene nanoribbon arrays lithographically, and used the gas phase etching chemistry to narrow the ribbons down to <10 nm. For the first time, a high on/off ratio up to approximately 10(4) was achieved at room temperature for field-effect transistors built with sub-5-nm-wide graphene nanoribbon semiconductors derived from lithographic patterning and narrowing. Our controlled etching method opens up a chemical way to control the size of various graphene nano-structures beyond the capability of top-down lithography.

  View details for DOI 10.1038/NCHEM.719

  View details for Web of Science ID 000280199500017

  View details for PubMedID 20651729

• Edge magnetotransport fingerprints in disordered graphene nanoribbons PHYSICAL REVIEW B Poumirol, J., Cresti, A., Roche, S., Escoffier, W., Goiran, M., Wang, X., Li, X., Dai, H., Raquet, B. 2010; 82 (4)

  View details for DOI 10.1103/PhysRevB.82.041413

  View details for Web of Science ID 000280475200002

• Ni(OH)(2) Nanoplates Grown on Graphene as Advanced Electrochemical Pseudocapacitor Materials JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Wang, H., Casalongue, H. S., Liang, Y., Dai, H. 2010; 132 (21): 7472-7477

  Abstract

  Ni(OH)(2) nanocrystals grown on graphene sheets with various degrees of oxidation are investigated as electrochemical pseudocapacitor materials for potential energy storage applications. Single-crystalline Ni(OH)(2) hexagonal nanoplates directly grown on lightly oxidized, electrically conducting graphene sheets (GS) exhibit a high specific capacitance of approximately 1335 F/g at a charge and discharge current density of 2.8 A/g and approximately 953 F/g at 45.7 A/g with excellent cycling ability. The high specific capacitance and remarkable rate capability are promising for applications in supercapacitors with both high energy and power densities. A simple physical mixture of pre-synthesized Ni(OH)(2) nanoplates and graphene sheets shows lower specific capacitance, highlighting the importance of direct growth of nanomaterials on graphene to impart intimate interactions and efficient charge transport between the active nanomaterials and the conducting graphene network. Single-crystalline Ni(OH)(2) nanoplates directly grown on graphene sheets also significantly outperform small Ni(OH)(2) nanoparticles grown on heavily oxidized, electrically insulating graphite oxide (GO), suggesting that the electrochemical performance of these composites is dependent on the quality of graphene substrates and the morphology and crystallinity of the nanomaterials grown on top. These results suggest the importance of rational design and synthesis of graphene-based nanocomposite materials for high-performance energy applications.

  View details for DOI 10.1021/ja102267j

  View details for PubMedID 20443559

• Aligned graphene nanoribbons and crossbars from unzipped carbon nanotubes NANO RESEARCH Jiao, L., Zhang, L., Ding, L., Liu, J., Dai, H. 2010; 3 (6): 387-394

  View details for DOI 10.1007/s12274-010-1043-z

  View details for Web of Science ID 000278624100001

• Ultrahigh Sensitivity Carbon Nanotube Agents for Photoacoustic Molecular Imaging in Living Mice NANO LETTERS de la Zerda, A., Liu, Z., Bodapati, S., Teed, R., Vaithilingam, S., Khuri-Yakub, B. T., Chen, X., Dai, H., Gambhir, S. S. 2010; 10 (6): 2168-2172

  Abstract

  Photoacoustic imaging is an emerging modality that overcomes to a great extent the resolution and depth limitations of optical imaging while maintaining relatively high-contrast. However, since many diseases will not manifest an endogenous photoacoustic contrast, it is essential to develop exogenous photoacoustic contrast agents that can target diseased tissue(s). Here we present a novel photoacoustic contrast agent, Indocyanine Green dye-enhanced single walled carbon nanotube (SWNT-ICG). We conjugated this contrast agent with cyclic Arg-Gly-Asp (RGD) peptides to molecularly target the alpha(v)beta(3) integrins, which are associated with tumor angiogenesis. Intravenous administration of this tumor-targeted contrast agent to tumor-bearing mice showed significantly higher photoacoustic signal in the tumor than in mice injected with the untargeted contrast agent. The new contrast agent gave a markedly 300 times higher photoacoustic contrast in living tissues than previously reported SWNTs, leading to subnanomolar sensitivities. Finally, we show that the new contrast agent can detect approximately 20 times fewer cancer cells than previously reported SWNTs.

  View details for DOI 10.1021/nl100890d

  View details for Web of Science ID 000278449200033

  View details for PubMedID 20499887

  View details for PubMedCentralID PMC2893026

• Facile synthesis of high-quality graphene nanoribbons NATURE NANOTECHNOLOGY Jiao, L., Wang, X., Diankov, G., Wang, H., Dai, H. 2010; 5 (5): 321-325

  Abstract

  Graphene nanoribbons have attracted attention because of their novel electronic and spin transport properties, and also because nanoribbons less than 10 nm wide have a bandgap that can be used to make field-effect transistors. However, producing nanoribbons of very high quality, or in high volumes, remains a challenge. Here, we show that pristine few-layer nanoribbons can be produced by unzipping mildly gas-phase oxidized multiwalled carbon nanotubes using mechanical sonication in an organic solvent. The nanoribbons are of very high quality, with smooth edges (as seen by high-resolution transmission electron microscopy), low ratios of disorder to graphitic Raman bands, and the highest electrical conductance and mobility reported so far (up to 5e(2)/h and 1,500 cm(2) V(-1) s(-1) for ribbons 10-20 nm in width). Furthermore, at low temperatures, the nanoribbons show phase-coherent transport and Fabry-Perot interference, suggesting minimal defects and edge roughness. The yield of nanoribbons is approximately 2% of the starting raw nanotube soot material, significantly higher than previous methods capable of producing high-quality narrow nanoribbons. The relatively high-yield synthesis of pristine graphene nanoribbons will make these materials easily accessible for a wide range of fundamental and practical applications.

  View details for DOI 10.1038/NNANO.2010.54

  View details for PubMedID 20364133

• Nanocrystal Growth on Graphene with Various Degrees of Oxidation JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Wang, H., Robinson, J. T., Diankov, G., Dai, H. 2010; 132 (10): 3270-?

  Abstract

  We show a general two-step method for growing hydroxide and oxide nanocrystals of the iron family elements (Ni, Co, Fe) on graphene with two degrees of oxidation. Drastically different nanocrystal growth behaviors were observed on low-oxidation graphene sheets (GS) and highly oxidized graphite oxide (GO) in hydrothermal reactions. Small particles precoated on GS with few oxygen-containing surface groups diffused and recrystallized into single-crystalline Ni(OH)(2) hexagonal nanoplates or Fe(2)O(3) nanorods with well-defined morphologies. In contrast, particles precoated on GO were pinned by the high-concentration oxygen groups and defects on GO without recrystallization into well-defined shapes. Adjusting the reaction temperature can be included to further control materials grown on graphene. For materials with weak interactions with graphene, increasing the reaction temperature can lead to diffusion and recrystallization of surface species into larger crystals, even on highly oxidized and defective GO. Our results suggest an interesting new approach for controlling the morphology of nanomaterials grown on graphene by tuning the surface chemistry of graphene substrates used for crystal nucleation and growth.

  View details for DOI 10.1021/ja100329d

  View details for PubMedID 20166667

• Multiplexed Five-Color Molecular Imaging of Cancer Cells and Tumor Tissues with Carbon Nanotube Raman Tags in the Near-Infrared NANO RESEARCH Liu, Z., Tabakman, S., Sherlock, S., Li, X., Chen, Z., Jiang, K., Fan, S., Dai, H. 2010; 3 (3): 222-233

  Abstract

  Single-walled carbon nanotubes (SWNTs) with five different C13/C12 isotope compositions and well-separated Raman peaks have been synthesized and conjugated to five targeting ligands in order to impart molecular specificity. Multiplexed Raman imaging of live cells has been carried out by highly specific staining of cells with a five-color mixture of SWNTs. Ex vivo multiplexed Raman imaging of tumor samples uncovers a surprising up-regulation of epidermal growth factor receptor (EGFR) on LS174T colon cancer cells from cell culture to in vivo tumor growth. This is the first time five-color multiplexed molecular imaging has been performed in the near-infrared (NIR) region under a single laser excitation. Near zero interfering background of imaging is achieved due to the sharp Raman peaks unique to nanotubes over the low, smooth autofluorescence background of biological species.

  View details for DOI 10.1007/s12274-010-1025-1

  View details for Web of Science ID 000275754900008

  View details for PubMedCentralID PMC3062899

• Projected Performance Advantage of Multilayer Graphene Nanoribbons as a Transistor Channel Material NANO RESEARCH Ouyang, Y., Dai, H., Guo, J. 2010; 3 (1): 8-15

  View details for DOI 10.1007/s12274-010-1002-8

  View details for Web of Science ID 000273940100002

• High-Contrast In Vivo Visualization of Microvessels Using Novel FeCo/GC Magnetic Nanocrystals MAGNETIC RESONANCE IN MEDICINE Lee, J. H., Sherlock, S. P., Terashima, M., Kosuge, H., Suzuki, Y., Goodwin, A., Robinson, J., Seo, W. S., Liu, Z., Luong, R., McConnell, M. V., Nishimura, D. G., Dai, H. 2009; 62 (6): 1497-1509

  Abstract

  FeCo-graphitic carbon shell nanocrystals are a novel MRI contrast agent with unprecedented high per-metal-atom-basis relaxivity (r(1) = 97 mM(-1) sec(-1), r(2) = 400 mM(-1) sec(-1)) and multifunctional capabilities. While the conventional gadolinium-based contrast-enhanced angiographic magnetic MRI has proven useful for diagnosis of vascular diseases, its short circulation time and relatively low sensitivity render high-resolution MRI of morphologically small vascular structures such as those involved in collateral, arteriogenic, and angiogenic vessel formation challenging. Here, by combining FeCo-graphitic carbon shell nanocrystals with high-resolution MRI technique, we demonstrate that such microvessels down to approximately 100 mum can be monitored in high contrast and noninvasively using a conventional 1.5-T clinical MRI system, achieving a diagnostic imaging standard approximating that of the more invasive X-ray angiography. Preliminary in vitro and in vivo toxicity study results also show no sign of toxicity.

  View details for DOI 10.1002/mrm.22132

  View details for PubMedID 19859938

• Simultaneous Nitrogen Doping and Reduction of Graphene Oxide JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Li, X., Wang, H., Robinson, J. T., Sanchez, H., Diankov, G., Dai, H. 2009; 131 (43): 15939-15944

  Abstract

  We developed a simple chemical method to obtain bulk quantities of N-doped, reduced graphene oxide (GO) sheets through thermal annealing of GO in ammonia. X-ray photoelectron spectroscopy (XPS) study of GO sheets annealed at various reaction temperatures reveals that N-doping occurs at a temperature as low as 300 degrees C, while the highest doping level of approximately 5% N is achieved at 500 degrees C. N-doping is accompanied by the reduction of GO with decreases in oxygen levels from approximately 28% in as-made GO down to approximately 2% in 1100 degrees C NH(3) reacted GO. XPS analysis of the N binding configurations of doped GO finds pyridinic N in the doped samples, with increased quaternary N (N that replaced the carbon atoms in the graphene plane) in GO annealed at higher temperatures (> or = 900 degrees C). Oxygen groups in GO were found responsible for reactions with NH(3) and C-N bond formation. Prereduced GO with fewer oxygen groups by thermal annealing in H(2) exhibits greatly reduced reactivity with NH(3) and a lower N-doping level. Electrical measurements of individual GO sheet devices demonstrate that GO annealed in NH(3) exhibits higher conductivity than those annealed in H(2), suggesting more effective reduction of GO by annealing in NH(3) than in H(2), consistent with XPS data. The N-doped reduced GO shows clearly n-type electron doping behavior with the Dirac point (DP) at negative gate voltages in three terminal devices. Our method could lead to the synthesis of bulk amounts of N-doped, reduced GO sheets useful for various practical applications.

  View details for DOI 10.1021/ja907098f

  View details for PubMedID 19817436

• Carbon Nanotubes Allow Fluorescence Imaging of Macrophages in Mouse Carotid Atherosclerosis 82nd National Conference and Exhibitions and Scientific Sessions of the American-Heart-Association Kosuge, H., Terashima, M., Sherlock, S., Kitagawa, T., Dai, H., McConnell, M. V. LIPPINCOTT WILLIAMS & WILKINS. 2009: S1113–S1113

  View details for Web of Science ID 000271831504081

• Hierarchy of Electronic Properties of Chemically Derived and Pristine Graphene Probed by Microwave Imaging NANO LETTERS Kundhikanjana, W., Lai, K., Wang, H., Dai, H., Kelly, M. A., Shen, Z. 2009; 9 (11): 3762-3765

  Abstract

  Local electrical imaging using microwave impedance microscope is performed on graphene in different modalities, yielding a rich hierarchy of the local conductivity. The low-conductivity graphite oxide and its derivatives show significant electronic inhomogeneity. For the conductive chemical graphene, the residual defects lead to a systematic reduction of the microwave signals. In contrast, the signals on pristine graphene agree well with a lumped-element circuit model. The local impedance information can also be used to verify the electrical contact between overlapped graphene pieces.

  View details for DOI 10.1021/nl901949z

  View details for PubMedID 19678669

• A route to brightly fluorescent carbon nanotubes for near-infrared imaging in mice NATURE NANOTECHNOLOGY Welsher, K., Liu, Z., Sherlock, S. P., Robinson, J. T., Chen, Z., Daranciang, D., Dai, H. 2009; 4 (11): 773-780

  Abstract

  The near-infrared photoluminescence intrinsic to semiconducting single-walled carbon nanotubes is ideal for biological imaging owing to the low autofluorescence and deep tissue penetration in the near-infrared region beyond 1 microm. However, biocompatible single-walled carbon nanotubes with high quantum yield have been elusive. Here, we show that sonicating single-walled carbon nanotubes with sodium cholate, followed by surfactant exchange to form phospholipid-polyethylene glycol coated nanotubes, produces in vivo imaging agents that are both bright and biocompatible. The exchange procedure is better than directly sonicating the tubes with the phospholipid-polyethylene glycol, because it results in less damage to the nanotubes and improves the quantum yield. We show whole-animal in vivo imaging using an InGaAs camera in the 1-1.7 microm spectral range by detecting the intrinsic near-infrared photoluminescence of the 'exchange' single-walled carbon nanotubes at a low dose (17 mg l(-1) injected dose). The deep tissue penetration and low autofluorescence background allowed high-resolution intravital microscopy imaging of tumour vessels beneath thick skin.

  View details for DOI 10.1038/NNANO.2009.294

  View details for Web of Science ID 000272413500022

  View details for PubMedID 19893526

  View details for PubMedCentralID PMC2834239

• ANYL 250-Carbon nanotube as Raman tag for biomolecule sensing Chen, Z., Tabakman, S., Dai, H. AMER CHEMICAL SOC. 2009

  View details for Web of Science ID 000207861901278

• Chemically derived graphene nanoribbons and large-scale high quality graphene sheets: Synthesis, assembly, and devices Li, X., Wang, X., Wang, H., Dai, H. AMER CHEMICAL SOC. 2009

  View details for Web of Science ID 000207861909299

• COLL 346-Brightly fluorescent carbon nanotubes for near infrared imaging in mice Welsher, K., Liu, Z., Sherlock, S., Robinson, J., Chen, Z., Daranciang, D., Dai, H. AMER CHEMICAL SOC. 2009

  View details for Web of Science ID 000207861903526

• Chemically derived graphene nanoribbons and large-scale high quality graphene sheets: Synthesis, assembly, and devices Li, X., Dai, H. AMER CHEMICAL SOC. 2009: 25–25

  View details for Web of Science ID 000207861900024

• Solvothermal Reduction of Chemically Exfoliated Graphene Sheets JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Wang, H., Robinson, J. T., Li, X., Dai, H. 2009; 131 (29): 9910-?

  Abstract

  We have developed a solvothermal reduction method that affords more effective reduction of chemically derived graphene sheets and graphite oxide than low-temperature reduction methods. Solvothermal reduction removed oxygen and defects from graphene sheets, increased the size of sp(2) domains, and produced materials that were as conducting as pristine graphene and exhibited clear intrinsic Dirac behavior.

  View details for DOI 10.1021/ja904251p

  View details for PubMedID 19580268

• N-Doping of Graphene Through Electrothermal Reactions with Ammonia SCIENCE Wang, X., Li, X., Zhang, L., Yoon, Y., Weber, P. K., Wang, H., Guo, J., Dai, H. 2009; 324 (5928): 768-771

  Abstract

  Graphene is readily p-doped by adsorbates, but for device applications, it would be useful to access the n-doped material. Individual graphene nanoribbons were covalently functionalized by nitrogen species through high-power electrical joule heating in ammonia gas, leading to n-type electronic doping consistent with theory. The formation of the carbon-nitrogen bond should occur mostly at the edges of graphene where chemical reactivity is high. X-ray photoelectron spectroscopy and nanometer-scale secondary ion mass spectroscopy confirm the carbon-nitrogen species in graphene thermally annealed in ammonia. We fabricated an n-type graphene field-effect transistor that operates at room temperature.

  View details for DOI 10.1126/science.1170335

  View details for PubMedID 19423822

• Narrow graphene nanoribbons from carbon nanotubes NATURE Jiao, L., Zhang, L., Wang, X., Diankov, G., Dai, H. 2009; 458 (7240): 877-880

  Abstract

  Graphene nanoribbons (GNRs) are materials with properties distinct from those of other carbon allotropes. The all-semiconducting nature of sub-10-nm GNRs could bypass the problem of the extreme chirality dependence of the metal or semiconductor nature of carbon nanotubes (CNTs) in future electronics. Currently, making GNRs using lithographic, chemical or sonochemical methods is challenging. It is difficult to obtain GNRs with smooth edges and controllable widths at high yields. Here we show an approach to making GNRs by unzipping multiwalled carbon nanotubes by plasma etching of nanotubes partly embedded in a polymer film. The GNRs have smooth edges and a narrow width distribution (10-20 nm). Raman spectroscopy and electrical transport measurements reveal the high quality of the GNRs. Unzipping CNTs with well-defined structures in an array will allow the production of GNRs with controlled widths, edge structures, placement and alignment in a scalable fashion for device integration.

  View details for DOI 10.1038/nature07919

  View details for Web of Science ID 000265182500040

  View details for PubMedID 19370031

• PEG Branched Polymer for Functionalization of Nanomaterials with Ultralong Blood Circulation JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Prencipe, G., Tabakman, S. M., Welsher, K., Liu, Z., Goodwin, A. P., Zhang, L., Henry, J., Dai, H. 2009; 131 (13): 4783-4787

  Abstract

  Nanomaterials have been actively pursued for biological and medical applications in recent years. Here, we report the synthesis of several new poly(ethylene glycol) grafted branched polymers for functionalization of various nanomaterials including carbon nanotubes, gold nanoparticles (NPs), and gold nanorods (NRs), affording high aqueous solubility and stability for these materials. We synthesize different surfactant polymers based upon poly(gamma-glutamic acid) (gammaPGA) and poly(maleic anhydride-alt-1-octadecene) (PMHC18). We use the abundant free carboxylic acid groups of gammaPGA for attaching lipophilic species such as pyrene or phospholipid, which bind to nanomaterials via robust physisorption. Additionally, the remaining carboxylic acids on gammaPGA or the amine-reactive anhydrides of PMHC18 are then PEGylated, providing extended hydrophilic groups, affording polymeric amphiphiles. We show that single-walled carbon nanotubes (SWNTs), Au NPs, and NRs functionalized by the polymers exhibit high stability in aqueous solutions at different pH values, at elevated temperatures, and in serum. Moreover, the polymer-coated SWNTs exhibit remarkably long blood circulation (t(1/2) = 22.1 h) upon intravenous injection into mice, far exceeding the previous record of 5.4 h. The ultralong blood circulation time suggests greatly delayed clearance of nanomaterials by the reticuloendothelial system (RES) of mice, a highly desired property for in vivo applications of nanomaterials, including imaging and drug delivery.

  View details for DOI 10.1021/ja809086q

  View details for PubMedID 19173646

• Chemical Self-Assembly of Graphene Sheets NANO RESEARCH Wang, H., Wang, X., Li, X., Dai, H. 2009; 2 (4): 336-342

  View details for DOI 10.1007/s12274-009-9031-x

  View details for Web of Science ID 000273939200007

• Optical Characterizations and Electronic Devices of Nearly Pure (10,5) Single-Walled Carbon Nanotubes JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Zhang, L., Tu, X., Welsher, K., Wang, X., Zheng, M., Dai, H. 2009; 131 (7): 2454-?

  Abstract

  It remains an elusive goal to achieve high-performance single-walled carbon nanotube (SWNT) field-effect transistors (FETs) composed of only single-chirality SWNTs. Many separation mechanisms have been devised and various degrees of separation demonstrated, yet it is still difficult to reach the goal of total fractionation of a given nanotube mixture into its single-chirality components. Chromatography has been reported to separate small SWNTs (diameter < or = 0.9 nm) according to their diameter, chirality, and length. The separation efficiency decreased with increasing tube diameter when the ssDNA sequence d(GT)(n) (n = 10-45) was used. Here we report our results on the separation of single-chirality (10,5) SWNTs (diameter = 1.03 nm) from HiPco tubes using ion-exchange chromatography. The separation efficiency was improved by using the new DNA sequence (TTTA)(3)T, which can recognize SWNTs with the specific chirality (10,5). The chirality of the separated tubes was examined by optical absorption, Raman, photoluminescence excitation/emission, and electrical transport measurements. All of the spectroscopic methods gave a single peak of (10,5) tubes. The purity was 99% according to the electrical measurement. The FETs composed of separated SWNTs in parallel gave an I(on)/I(off) ratio up to 10(6) due to the single-chirality-enriched (10,5) tubes. This is the first time that SWNT FETs with single-chirality SWNTs have been achieved. The chromatography method has the potential to separate even larger diameter semiconducting SWNTs from other starting materials to further improve the performance of the SWNT FETs.

  View details for DOI 10.1021/ja8096674

  View details for Web of Science ID 000263576100018

  View details for PubMedID 19193007

• Carbon Nanotubes in Biology and Medicine: In vitro and in vivo Detection, Imaging and Drug Delivery NANO RESEARCH Liu, Z., Tabakman, S., Welsher, K., Dai, H. 2009; 2 (2): 85-120

  Abstract

  Carbon nanotubes exhibit many unique intrinsic physical and chemical properties and have been intensively explored for biological and biomedical applications in the past few years. In this comprehensive review, we summarize the main results from our and other groups in this field and clarify that surface functionalization is critical to the behavior of carbon nanotubes in biological systems. Ultrasensitive detection of biological species with carbon nanotubes can be realized after surface passivation to inhibit the non-specific binding of biomolecules on the hydrophobic nanotube surface. Electrical nanosensors based on nanotubes provide a label-free approach to biological detection. Surface-enhanced Raman spectroscopy of carbon nanotubes opens up a method of protein microarray with detection sensitivity down to 1 fmol/L. In vitro and in vivo toxicity studies reveal that highly water soluble and serum stable nanotubes are biocompatible, nontoxic, and potentially useful for biomedical applications. In vivo biodistributions vary with the functionalization and possibly also size of nanotubes, with a tendency to accumulate in the reticuloendothelial system (RES), including the liver and spleen, after intravenous administration. If well functionalized, nanotubes may be excreted mainly through the biliary pathway in feces. Carbon nanotube-based drug delivery has shown promise in various In vitro and in vivo experiments including delivery of small interfering RNA (siRNA), paclitaxel and doxorubicin. Moreover, single-walled carbon nanotubes with various interesting intrinsic optical properties have been used as novel photoluminescence, Raman, and photoacoustic contrast agents for imaging of cells and animals. Further multidisciplinary explorations in this field may bring new opportunities in the realm of biomedicine.

  View details for DOI 10.1007/s12274-009-9009-8

  View details for Web of Science ID 000273939000001

  View details for PubMedCentralID PMC2824900

• Carbon Nanotubes in Biology and Medicine: In vitro and in vivo Detection, Imaging and Drug Delivery. Nano research Liu, Z., Tabakman, S., Welsher, K., Dai, H. 2009; 2 (2): 85-120

  Abstract

  Carbon nanotubes exhibit many unique intrinsic physical and chemical properties and have been intensively explored for biological and biomedical applications in the past few years. In this comprehensive review, we summarize the main results from our and other groups in this field and clarify that surface functionalization is critical to the behavior of carbon nanotubes in biological systems. Ultrasensitive detection of biological species with carbon nanotubes can be realized after surface passivation to inhibit the non-specific binding of biomolecules on the hydrophobic nanotube surface. Electrical nanosensors based on nanotubes provide a label-free approach to biological detection. Surface-enhanced Raman spectroscopy of carbon nanotubes opens up a method of protein microarray with detection sensitivity down to 1 fmol/L. In vitro and in vivo toxicity studies reveal that highly water soluble and serum stable nanotubes are biocompatible, nontoxic, and potentially useful for biomedical applications. In vivo biodistributions vary with the functionalization and possibly also size of nanotubes, with a tendency to accumulate in the reticuloendothelial system (RES), including the liver and spleen, after intravenous administration. If well functionalized, nanotubes may be excreted mainly through the biliary pathway in feces. Carbon nanotube-based drug delivery has shown promise in various In vitro and in vivo experiments including delivery of small interfering RNA (siRNA), paclitaxel and doxorubicin. Moreover, single-walled carbon nanotubes with various interesting intrinsic optical properties have been used as novel photoluminescence, Raman, and photoacoustic contrast agents for imaging of cells and animals. Further multidisciplinary explorations in this field may bring new opportunities in the realm of biomedicine.

  View details for DOI 10.1007/s12274-009-9009-8

  View details for PubMedID 20174481

  View details for PubMedCentralID PMC2824900

• Phospholipid-Dextran with a Single Coupling Point: A Useful Amphiphile for Functionalization of Nanomaterials JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Goodwin, A. P., Tabakman, S. M., Welsher, K., Sherlock, S. P., Prencipe, G., Dai, H. 2009; 131 (1): 289-296

  Abstract

  Nanomaterials hold much promise for biological applications, but they require appropriate functionalization to provide biocompatibility in biological environments. For noncovalent functionalization with biocompatible polymers, the polymer must also remain attached to the nanomaterial after removal of its excess to mimic the high-dilution conditions of administration in vivo. Reported here are the synthesis and utilization of singly substituted conjugates of dextran and a phospholipid (dextran-DSPE) as stable coatings for nanomaterials. Suspensions of single-walled carbon nanotubes were found not only to be stable to phosphate buffered saline (PBS), serum, and a variety of pH's after excess polymer removal, but also to provide brighter photoluminescence than carbon nanotubes suspended by poly(ethylene glycol)-DSPE. In addition, both gold nanoparticles (AuNPs) and gold nanorods (AuNRs) were found to maintain their dispersion and characteristic optical absorbance after transfer into dextran-DSPE and were obtained in much better yield than similar suspensions with PEG-phospholipid and commonly used thiol-PEG. These suspensions were also stable to PBS, serum, and a variety of pH's after removal of excess polymer. dextran-DSPE thus shows great promise as a general surfactant material for the functionalization of a variety of nanomaterials, which could facilitate future biological applications.

  View details for DOI 10.1021/ja807307e

  View details for Web of Science ID 000262483100060

  View details for PubMedID 19061329

  View details for PubMedCentralID PMC2827334

• Enhanced Sensitivity Carbon Nanotubes as Targeted Photoacoustic Molecular Imaging Agents Conference on Photons Plus Ultrasound - Imaging and Sensing 2009 de la Zerda, A., Liu, Z., Zavaleta, C., Bodapati, S., Teed, R., Vaithilingam, S., Ma, T., Oralkan, O., Chen, X., Khuri-Yakub, B. T., Dai, H., Gambhir, S. S. SPIE-INT SOC OPTICAL ENGINEERING. 2009

  View details for DOI 10.1117/12.809601

  View details for Web of Science ID 000285714100080

• Multilayer Graphene Nanoribbon for 3D Stacking of the Transistor Channel Ouyang, Y., Dai, H., Guo, J., IEEE IEEE. 2009: 833-+

  View details for Web of Science ID 000279343900214

• Separation of Nanoparticles in a Density Gradient: FeCo@C and Gold Nanocrystals ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Sun, X., Tabakman, S. M., Seo, W., Zhang, L., Zhang, G., Sherlock, S., Bai, L., Dai, H. 2009; 48 (5): 939-942

  View details for DOI 10.1002/anie.200805047

  View details for Web of Science ID 000263082200016

  View details for PubMedID 19107884

  View details for PubMedCentralID PMC2656675

• Preparation of carbon nanotube bioconjugates for biomedical applications NATURE PROTOCOLS Liu, Z., Tabakman, S. M., Chen, Z., Dai, H. 2009; 4 (9): 1372-1382

  Abstract

  Biomedical applications of carbon nanotubes have attracted much attention in recent years. Here, we summarize our previously developed protocols for functionalization and bioconjugation of single-walled carbon nanotubes (SWNTs) for various biomedical applications including biological imaging; using nanotubes as Raman, photoluminescence and photoacoustic labels; sensing using nanotubes as Raman tags and drug delivery. Sonication of SWNTs in solutions of phospholipid-polyethylene glycol (PL-PEG) is our most commonly used protocol of SWNT functionalization. Compared with other frequently used covalent strategies, our non-covalent functionalization protocol largely retains the intrinsic optical properties of SWNTs, which are useful in various biological imaging and sensing applications. Functionalized SWNTs are conjugated with targeting ligands, including peptides and antibodies for specific cell labeling in vitro or tumor targeting in vivo. Radio labels are introduced for tracking and imaging of SWNTs in real time in vivo. Moreover, SWNTs can be conjugated with small interfering RNA (siRNA) or loaded with chemotherapy drugs for drug delivery. These procedures take various times ranging from 1 to 5 d.

  View details for DOI 10.1038/nprot.2009.146

  View details for Web of Science ID 000270601700014

  View details for PubMedID 19730421

  View details for PubMedCentralID PMC2853228

• Supramolecular Stacking of Doxorubicin on Carbon Nanotubes for In Vivo Cancer Therapy ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Liu, Z., Fan, A. C., Rakhra, K., Sherlock, S., Goodwin, A., Chen, X., Yang, Q., Felsher, D. W., Dai, H. 2009; 48 (41): 7668-7672

  View details for DOI 10.1002/anie.200902612

  View details for PubMedID 19760685

• Photoacoustic Molecular Imaging using Single Walled Carbon Nanotubes in Living Mice Conference on Photons Plus Ultrasound - Imaging and Sensing 2009 de la Zerda, A., Zavaleta, C., Keren, S., Vaithilingam, S., Bodapati, S., Teed, R., Liu, Z., Levi, J., Smith, B. R., Ma, T., Oralkan, O., Cheng, Z., Chen, X., Dai, H., Khuri-Yakub, B. T., Gambhir, S. S. SPIE-INT SOC OPTICAL ENGINEERING. 2009

  View details for DOI 10.1117/12.806497

  View details for Web of Science ID 000285714100066

• Synthesis of Ultrasmall Ferromagnetic Face-Centered Tetragonal FePt-Graphite Core-Shell Nanocrystals SMALL Seo, W. S., Kim, S. M., Kim, Y., Sun, X., Dai, H. 2008; 4 (11): 1968-1971

  View details for DOI 10.1002/smll.200800257

  View details for Web of Science ID 000261230400018

  View details for PubMedID 18752210

  View details for PubMedCentralID PMC2824537

• Protein microarrays with carbon nanotubes as multicolor Raman labels NATURE BIOTECHNOLOGY Chen, Z., Tabakman, S. M., Goodwin, A. P., Kattah, M. G., Daranciang, D., Wang, X., Zhang, G., Li, X., Liu, Z., Utz, P. J., Jiang, K., Fan, S., Dai, H. 2008; 26 (11): 1285-1292

  Abstract

  The current sensitivity of standard fluorescence-based protein detection limits the use of protein arrays in research and clinical diagnosis. Here, we use functionalized, macromolecular single-walled carbon nanotubes (SWNTs) as multicolor Raman labels for highly sensitive, multiplexed protein detection in an arrayed format. Unlike fluorescence methods, Raman detection benefits from the sharp scattering peaks of SWNTs with minimal background interference, affording a high signal-to-noise ratio needed for ultra-sensitive detection. When combined with surface-enhanced Raman scattering substrates, the strong Raman intensity of SWNT tags affords protein detection sensitivity in sandwich assays down to 1 fM--a three-order-of-magnitude improvement over most reports of fluorescence-based detection. We use SWNT Raman tags to detect human autoantibodies against proteinase 3, a biomarker for the autoimmune disease Wegener's granulomatosis, diluted up to 10(7)-fold in 1% human serum. SWNT Raman tags are not subject to photobleaching or quenching. By conjugating different antibodies to pure (12)C and (13)C SWNT isotopes, we demonstrate multiplexed two-color SWNT Raman-based protein detection.

  View details for DOI 10.1038/nbt.1501

  View details for Web of Science ID 000260832200024

  View details for PubMedID 18953353

• Multiplexed multicolor Raman imaging of live cells with isotopically modified single walled carbon nanotubes JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Liu, Z., Li, X., Tabakman, S. M., Jiang, K., Fan, S., Dai, H. 2008; 130 (41): 13540-?

  Abstract

  We show that single walled carbon nanotubes (SWNTs) with different isotope compositions exhibit distinct Raman G-band peaks and can be used for multiplexed multicolor Raman imaging of biological systems. Cancer cells with specific receptors are selectively labeled with three differently "colored" SWNTs conjugated with various targeting ligands including Herceptin (anti-Her2), Erbitux (anti-Her1), and RGD peptide, allowing for multicolor Raman imaging of cells in a multiplexed manner. SWNT Raman signals are highly robust against photobleaching, allowing long-term imaging and tracking. With narrow peak features, SWNT Raman signals are easily differentiated from the autofluorescence background. The SWNT Raman excitation and scattering photons are in the near-infrared region, which is the most transparent optical window for biological systems in vitro and in vivo. Thus, SWNTs are novel Raman tags promising for multiplexed biological detection and imaging.

  View details for DOI 10.1021/ja806242t

  View details for Web of Science ID 000259924000017

  View details for PubMedID 18803379

  View details for PubMedCentralID PMC2617744

• Converting Metallic Single-Walled Carbon Nanotnbes into Semiconductors by Boron/Nitrogen Co-Doping ADVANCED MATERIALS Xu, Z., Lu, W., Wang, W., Gu, C., Liu, K., Bai, X., Wang, E., Dai, H. 2008; 20 (19): 3615-?

  View details for DOI 10.1002/adma.200800830

  View details for Web of Science ID 000260023900007

• Carbon nanotubes as photoacoustic molecular imaging agents in living mice NATURE NANOTECHNOLOGY de la Zerda, A., Zavaleta, C., Keren, S., Vaithilingam, S., Bodapati, S., Liu, Z., Levi, J., Smith, B. R., Ma, T., Oralkan, O., Cheng, Z., Chen, X., Dai, H., Khuri-Yakub, B. T., Gambhir, S. S. 2008; 3 (9): 557-562

  Abstract

  Photoacoustic imaging of living subjects offers higher spatial resolution and allows deeper tissues to be imaged compared with most optical imaging techniques. As many diseases do not exhibit a natural photoacoustic contrast, especially in their early stages, it is necessary to administer a photoacoustic contrast agent. A number of contrast agents for photoacoustic imaging have been suggested previously, but most were not shown to target a diseased site in living subjects. Here we show that single-walled carbon nanotubes conjugated with cyclic Arg-Gly-Asp (RGD) peptides can be used as a contrast agent for photoacoustic imaging of tumours. Intravenous administration of these targeted nanotubes to mice bearing tumours showed eight times greater photoacoustic signal in the tumour than mice injected with non-targeted nanotubes. These results were verified ex vivo using Raman microscopy. Photoacoustic imaging of targeted single-walled carbon nanotubes may contribute to non-invasive cancer imaging and monitoring of nanotherapeutics in living subjects.

  View details for DOI 10.1038/nnano.2008.231

  View details for Web of Science ID 000259013100014

  View details for PubMedID 18772918

  View details for PubMedCentralID PMC2562547

• Noninvasive Raman spectroscopy in living mice for evaluation of tumor targeting with carbon nanotubes NANO LETTERS Zavaleta, C., de la Zerda, A., Liu, Z., Keren, S., Cheng, Z., Schipper, M., Chen, X., Dai, H., Gambhir, S. S. 2008; 8 (9): 2800-2805

  Abstract

  An optimized noninvasive Raman microscope was used to evaluate tumor targeting and localization of single walled carbon nanotubes (SWNTs) in mice. Raman images were acquired in two groups of tumor-bearing mice. The control group received plain-SWNTs, whereas the experimental group received tumor targeting RGD-SWNTs intravenously. Raman imaging commenced over the next 72 h and revealed increased accumulation of RGD-SWNTs in tumor ( p < 0.05) as opposed to plain-SWNTs. These results support the development of a new preclinical Raman imager.

  View details for DOI 10.1021/nl801362a

  View details for Web of Science ID 000259140200034

  View details for PubMedID 18683988

  View details for PubMedCentralID PMC2910584

• Nano-Graphene Oxide for Cellular Imaging and Drug Delivery NANO RESEARCH Sun, X., Liu, Z., Welsher, K., Robinson, J. T., Goodwin, A., Zaric, S., Dai, H. 2008; 1 (3): 203-212

  Abstract

  Two-dimensional graphene offers interesting electronic, thermal, and mechanical properties that are currently being explored for advanced electronics, membranes, and composites. Here we synthesize and explore the biological applications of nano-graphene oxide (NGO), i.e., single-layer graphene oxide sheets down to a few nanometers in lateral width. We develop functionalization chemistry in order to impart solubility and compatibility of NGO in biological environments. We obtain size separated pegylated NGO sheets that are soluble in buffers and serum without agglomeration. The NGO sheets are found to be photoluminescent in the visible and infrared regions. The intrinsic photoluminescence (PL) of NGO is used for live cell imaging in the near-infrared (NIR) with little background. We found that simple physisorption via pi-stacking can be used for loading doxorubicin, a widely used cancer drug onto NGO functionalized with antibody for selective killing of cancer cells in vitro. Owing to its small size, intrinsic optical properties, large specific surface area, low cost, and useful non-covalent interactions with aromatic drug molecules, NGO is a promising new material for biological and medical applications.

  View details for DOI 10.1007/s12274-008-8021-8

  View details for Web of Science ID 000207467200003

  View details for PubMedCentralID PMC2834318

• Highly conducting graphene sheets and Langmuir-Blodgett films NATURE NANOTECHNOLOGY Li, X., Zhang, G., Bai, X., Sun, X., Wang, X., Wang, E., Dai, H. 2008; 3 (9): 538-542

  Abstract

  Graphene is an intriguing material with properties that are distinct from those of other graphitic systems. The first samples of pristine graphene were obtained by 'peeling off' and epitaxial growth. Recently, the chemical reduction of graphite oxide was used to produce covalently functionalized single-layer graphene oxide. However, chemical approaches for the large-scale production of highly conducting graphene sheets remain elusive. Here, we report that the exfoliation-reintercalation-expansion of graphite can produce high-quality single-layer graphene sheets stably suspended in organic solvents. The graphene sheets exhibit high electrical conductance at room and cryogenic temperatures. Large amounts of graphene sheets in organic solvents are made into large transparent conducting films by Langmuir-Blodgett assembly in a layer-by-layer manner. The chemically derived, high-quality graphene sheets could lead to future scalable graphene devices.

  View details for DOI 10.1038/nnano.2008.210

  View details for Web of Science ID 000259013100010

  View details for PubMedID 18772914

• Targeted single-wall carbon nanotube-mediated Pt(IV) prodrug delivery using folate as a homing device JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Dhar, S., Liu, Z., Thomale, J., Dai, H., Lippard, S. J. 2008; 130 (34): 11467-11476

  Abstract

  Most low-molecular-weight platinum anticancer drugs have short blood circulation times that are reflected in their reduced tumor uptake and intracellular DNA binding. A platinum(IV) complex of the formula c, c, t-[Pt(NH 3) 2Cl 2(O 2CCH 2CH 2CO 2H)(O 2CCH 2CH 2CONH-PEG-FA)] ( 1), containing a folate derivative (FA) at an axial position, was prepared and characterized. Folic acid offers a means of targeting human cells that highly overexpress the folate receptor (FR). Compound 1 was attached to the surface of an amine-functionalized single-walled carbon nanotube (SWNT-PL-PEG-NH 2) through multiple amide linkages to use the SWNTs as a "longboat delivery system" for the platinum warhead, carrying it to the tumor cell and releasing cisplatin upon intracellular reduction of Pt(IV) to Pt(II). The ability of SWNT tethered 1 to destroy selectively FR(+) vs FR(-) cells demonstrated its ability to target tumor cells that overexpress the FR on their surface. That the SWNTs deliver the folate-bearing Pt(IV) cargos into FR(+) cancer cells by endocytosis was demonstrated by the localization of fluorophore-labeled SWNTs using fluorescence microscopy. Once inside the cell, cisplatin, formed upon reductive release from the longboat oars, enters the nucleus and reacts with its target nuclear DNA, as determined by platinum atomic absorption spectroscopy of cell extracts. Formation of the major cisplatin 1,2-intrastrand d(GpG) cross-links on the nuclear DNA was demonstrated by use of a monoclonal antibody specific for this adduct. The SWNT-tethered compound 1 is the first construct in which both the targeting and delivery moieties have been incorporated into the same molecule; it is also the first demonstration that intracellular reduction of a Pt(IV) prodrug leads to the cis-{Pt((NH 3) 2} 1,2-intrastrand d(GpG) cross-link in nuclear DNA.

  View details for DOI 10.1021/ja803036e

  View details for Web of Science ID 000258660600046

  View details for PubMedID 18661990

  View details for PubMedCentralID PMC2536766

• PEGylated nanographene oxide for delivery of water-insoluble cancer drugs JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Liu, Z., Robinson, J. T., Sun, X., Dai, H. 2008; 130 (33): 10876-?

  Abstract

  It is known that many potent, often aromatic drugs are water insoluble, which has hampered their use for disease treatment. In this work, we functionalized nanographene oxide (NGO), a novel graphitic material, with branched polyethylene glycol (PEG) to obtain a biocompatible NGO-PEG conjugate stable in various biological solutions, and used them for attaching hydrophobic aromatic molecules including a camptothecin (CPT) analogue, SN38, noncovalently via pi-pi stacking. The resulting NGO-PEG-SN38 complex exhibited excellent water solubility while maintaining its high cancer cell killing potency similar to that of the free SN38 molecules in organic solvents. The efficacy of NGO-PEG-SN38 was far higher than that of irinotecan (CPT-11), a FDA-approved water soluble SN38 prodrug used for the treatment of colon cancer. Our results showed that graphene is a novel class of material promising for biological applications including future in vivo cancer treatment with various aromatic, low-solubility drugs.

  View details for DOI 10.1021/ja803688x

  View details for Web of Science ID 000258415900023

  View details for PubMedID 18661992

  View details for PubMedCentralID PMC2597374

• Drug delivery with carbon nanotubes for in vivo cancer treatment CANCER RESEARCH Liu, Z., Chen, K., Davis, C., Sherlock, S., Cao, Q., Chen, X., Dai, H. 2008; 68 (16): 6652-6660

  Abstract

  Chemically functionalized single-walled carbon nanotubes (SWNT) have shown promise in tumor-targeted accumulation in mice and exhibit biocompatibility, excretion, and little toxicity. Here, we show in vivo SWNT drug delivery for tumor suppression in mice. We conjugate paclitaxel (PTX), a widely used cancer chemotherapy drug, to branched polyethylene glycol chains on SWNTs via a cleavable ester bond to obtain a water-soluble SWNT-PTX conjugate. SWNT-PTX affords higher efficacy in suppressing tumor growth than clinical Taxol in a murine 4T1 breast cancer model, owing to prolonged blood circulation and 10-fold higher tumor PTX uptake by SWNT delivery likely through enhanced permeability and retention. Drug molecules carried into the reticuloendothelial system are released from SWNTs and excreted via biliary pathway without causing obvious toxic effects to normal organs. Thus, nanotube drug delivery is promising for high treatment efficacy and minimum side effects for future cancer therapy with low drug doses.

  View details for DOI 10.1158/0008-5472.CAN-08-1468

  View details for Web of Science ID 000258548200022

  View details for PubMedID 18701489

  View details for PubMedCentralID PMC2562710

• Complement activation by PEGylated single-walled carbon nanotubes is independent of C1q and alternative pathway turnover MOLECULAR IMMUNOLOGY Hamad, I., Hunter, A. C., Rutt, K. J., Liu, Z., Dai, H., Moghimi, S. M. 2008; 45 (14): 3797-3803

  Abstract

  We have investigated the interaction between long circulating poly(ethylene glycol)-stabilized single-walled carbon nanotubes (SWNTs) and the complement system. Aminopoly(ethylene glycol)(5000)-distearoylphosphatidylethanolamine (aminoPEG(5000)-DSPE) and methoxyPEG(5000)-DSPE coated as-grown HIPco SWNTs activated complement in undiluted normal human serum as reflected in significant rises in C4d and SC5b-9 levels, but not the alternative pathway split-product Bb, thus indicating activation exclusively through C4 cleavage. Studies in C2-depleted serum confirmed that PEGylated nanotube-mediated elevation of SC5b-9 was C4b2a convertase-dependent. With the aid of monoclonal antibodies against C1s and human serum depleted from C1q, nanotube-mediated complement activation in C1q-depleted serum was also shown to be independent of classical pathway. Nanotube-mediated C4d elevation in C1q-depleted serum, however, was inhibited by N-acetylglucosamine, Futhan (a broad-spectrum serine protease inhibitor capable of preventing complement activation through all three pathways) and anti-MASP-2 antibodies; this strongly suggests a role for activation of MASP-2 in subsequent C4 cleavage and assembly of C4b2a covertases. Intravenous injection of PEGylated nanotubes in some rats was associated with a significant rise in plasma thromboxane B2 levels, indicative of in vivo nanotube-mediated complement activation. The clinical implications of these observations are discussed.

  View details for DOI 10.1016/j.molimm.2008.05.020

  View details for Web of Science ID 000259473900013

  View details for PubMedID 18602161

  View details for PubMedCentralID PMC2824540

• Atomic layer deposition of metal oxides on pristine and functionalized graphene JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Wang, X., Tabakman, S. M., Dai, H. 2008; 130 (26): 8152-?

  Abstract

  We investigate atomic layer deposition (ALD) of metal oxide on pristine and functionalized graphene. On pristine graphene, ALD coating can only actively grow on edges and defect sites, where dangling bonds or surface groups react with ALD precursors. This affords a simple method to decorate and probe single defect sites in graphene planes. We used perylene tetracarboxylic acid (PTCA) to functionalize the graphene surface and selectively introduced densely packed surface groups on graphene. Uniform ultrathin ALD coating on PTCA graphene was achieved over a large area. The functionalization method could be used to integrate ultrathin high-kappa dielectrics in future graphene electronics.

  View details for DOI 10.1021/ja8023059

  View details for Web of Science ID 000257152800022

  View details for PubMedID 18529002

• Carrier scattering in graphene nanoribbon field-effect transistors APPLIED PHYSICS LETTERS Ouyang, Y., Wang, X., Dai, H., Guo, J. 2008; 92 (24)

  View details for DOI 10.1063/1.2949749

  View details for Web of Science ID 000256934900098

• Room-temperature all-semiconducting sub-10-nm graphene nanoribbon field-effect transistors PHYSICAL REVIEW LETTERS Wang, X., Ouyang, Y., Li, X., Wang, H., Guo, J., Dai, H. 2008; 100 (20)

  Abstract

  Sub-10 nm wide graphene nanoribbon field-effect transistors (GNRFETs) are studied systematically. All sub-10 nm GNRs afforded semiconducting FETs without exception, with Ion/Ioff ratio up to 10(6) and on-state current density as high as approximately 2000 microA/microm. We estimated carrier mobility approximately 200 cm2/V s and scattering mean free path approximately 10 nm in sub-10 nm GNRs. Scattering mechanisms by edges, acoustic phonon, and defects are discussed. The sub-10 nm GNRFETs are comparable to small diameter (d< or = approximately 1.2 nm) carbon nanotube FETs with Pd contacts in on-state current density and Ion/Ioff ratio, but have the advantage of producing all-semiconducting devices.

  View details for DOI 10.1103/PhysRevLett.100.206803

  View details for PubMedID 18518566

• Optical properties of ultrashort semiconducting single-walled carbon nanotube capsules down to sub-10 nm JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Sun, X., Zaric, S., Daranciang, D., Welsher, K., Lu, Y., Li, X., Dai, H. 2008; 130 (20): 6551-6555

  Abstract

  Single-walled carbon nanotubes (SWNTs) are typically long (greater than or approximately equal 100 nm) and have been well established as novel quasi one-dimensional systems with interesting electrical, mechanical, and optical properties. Here, quasi zero-dimensional SWNTs with finite lengths down to the molecular scale (7.5 nm in average) were obtained by length separation using a density gradient ultracentrifugation method. Different sedimentation rates of nanotubes with different lengths in a density gradient were taken advantage of to sort SWNTs according to length. Optical experiments on the SWNT fractions revealed that the UV-vis-NIR absorption and photoluminescence peaks of the ultrashort SWNTs blue-shift up to approximately 30 meV compared to long nanotubes, owing to quantum confinement effects along the length of ultrashort SWNTs. These nanotube capsules essentially correspond to SWNT quantum dots.

  View details for DOI 10.1021/ja8006929

  View details for Web of Science ID 000255854100049

  View details for PubMedID 18426207

• Peptide-coated nanotube-based biosensor for the detection of disease-specific autoantibodies in human serum BIOSENSORS & BIOELECTRONICS Drouvalakis, K. A., Bangsaruntip, S., Hueber, W., Kozar, L. G., Utz, P. J., Dai, H. 2008; 23 (10): 1413-1421

  Abstract

  We demonstrate a label-free peptide-coated carbon nanotube-based immunosensor for the direct assay of human serum. A rheumatoid arthritis (RA)-specific (cyclic citrulline-containing) peptide, was immobilized to functionalized single-walled carbon nanotubes deposited on a quartz crystal microbalance (QCM) sensing crystal. Serum from RA patients was used to probe these nanotube-based sensors, and antibody binding was detected by QCM sensing. Specific antibody binding was also determined by comparing the assay of two serum control groups (normal and diseased sera), and the native unmodified peptide. The sensitivity of the nanotube-based sensor (detection in the femtomol range) was higher than that of the established ELISA and recently described microarray assay systems, detecting 34.4 and 37.5% more RA patients with anti-citrullinated peptide antibodies than those found by ELISA and microarray, respectively. There was also an 18.4 and 19.6% greater chance of a negative test being a true indicator of a person not having RA than by either ELISA or microarray, respectively. The performance of our label-free biosensor enables its application in the direct assay of sera in research and diagnostics.

  View details for DOI 10.1016/j.bios.2007.11.022

  View details for Web of Science ID 000255793200001

  View details for PubMedID 18222083

  View details for PubMedCentralID PMC3418051

• Thermal properties of metal-coated vertically aligned single-wall nanotube arrays JOURNAL OF HEAT TRANSFER-TRANSACTIONS OF THE ASME Panzer, M. A., Zhang, G., Mann, D., Hu, X., Pop, E., Dai, H., Goodson, K. E. 2008; 130 (5)

  View details for DOI 10.1115/1.2885159

  View details for Web of Science ID 000255880300006

• PHYS 711-Carbon nanotubes chemistry for potential cancer therapy 235th American-Chemical-Society National Meeting Liu, Z., Dai, H. AMER CHEMICAL SOC. 2008

  View details for Web of Science ID 000271775109778

• A pilot toxicology study of single-walled carbon nanotubes in a small sample of mice NATURE NANOTECHNOLOGY Schipper, M. L., Nakayama-Ratchford, N., Davis, C. R., Kam, N. W., Chu, P., Liu, Z., Sun, X., Dai, H., Gambhir, S. S. 2008; 3 (4): 216-221

  Abstract

  Single-walled carbon nanotubes are currently under evaluation in biomedical applications, including in vivo delivery of drugs, proteins, peptides and nucleic acids (for gene transfer or gene silencing), in vivo tumour imaging and tumour targeting of single-walled carbon nanotubes as an anti-neoplastic treatment. However, concerns about the potential toxicity of single-walled carbon nanotubes have been raised. Here we examine the acute and chronic toxicity of functionalized single-walled carbon nanotubes when injected into the bloodstream of mice. Survival, clinical and laboratory parameters reveal no evidence of toxicity over 4 months. Upon killing, careful necropsy and tissue histology show age-related changes only. Histology and Raman microscopic mapping demonstrate that functionalized single-walled carbon nanotubes persisted within liver and spleen macrophages for 4 months without apparent toxicity. Although this is a preliminary study with a small group of animals, our results encourage further confirmation studies with larger groups of animals.

  View details for DOI 10.1038/nnano.2008.68

  View details for Web of Science ID 000254744300013

  View details for PubMedID 18654506

• Chemically derived, ultrasmooth graphene nanoribbon semiconductors SCIENCE Li, X., Wang, X., Zhang, L., Lee, S., Dai, H. 2008; 319 (5867): 1229-1232

  Abstract

  We developed a chemical route to produce graphene nanoribbons (GNR) with width below 10 nanometers, as well as single ribbons with varying widths along their lengths or containing lattice-defined graphene junctions for potential molecular electronics. The GNRs were solution-phase-derived, stably suspended in solvents with noncovalent polymer functionalization, and exhibited ultrasmooth edges with possibly well-defined zigzag or armchair-edge structures. Electrical transport experiments showed that, unlike single-walled carbon nanotubes, all of the sub-10-nanometer GNRs produced were semiconductors and afforded graphene field effect transistors with on-off ratios of about 10(7) at room temperature.

  View details for DOI 10.1126/science.1150878

  View details for Web of Science ID 000253530600039

  View details for PubMedID 18218865

• Assessment of chemically separated carbon nanotubes for nanoelectronics JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Zhang, L., Zaric, S., Tu, X., Wang, X., Zhao, W., Dai, H. 2008; 130 (8): 2686-2691

  Abstract

  It remains an elusive goal to obtain high performance single-walled carbon-nanotube (SWNT) electronics such as field effect transistors (FETs) composed of single- or few-chirality SWNTs, due to broad distributions in as-grown materials. Much progress has been made by various separation approaches to obtain materials enriched in metal or semiconducting nanotubes or even in single chiralties. However, research in validating SWNT separations by electrical transport measurements and building functional electronic devices has been scarce. Here, we performed length, diameter, and chirality separation of DNA functionalized HiPco SWNTs by chromatography methods, and we characterized the chiralities by photoluminescence excitation spectroscopy, optical absorption spectroscopy, and electrical transport measurements. The use of these combined methods provided deeper insight to the degree of separation than either technique alone. Separation of SWNTs by chirality and diameter occurred at varying degrees that decreased with increasing tube diameter. This calls for new separation methods capable of metallicity or chirality separation of large diameter SWNTs (in the approximately 1.5 nm range) needed for high performance nanoelectronics. With most of the separated fractions enriched in semiconducting SWNTs, nanotubes placed in parallel in short-channel (approximately 200 nm) electrical devices fail to produce FETs with high on/off switching, indicating incomplete elimination of metallic species. In rare cases with a certain separated SWNT fraction, we were able to fabricate FET devices composed of small-diameter, chemically separated SWNTs in parallel, with high on-/off-current (I(on)/I(off)) ratios up to 105 owing to semiconducting SWNTs with only a few (n,m) chiralities in the fraction. This was the first time that chemically separated SWNTs were used for short channel, all-semiconducting SWNT electronics dominant by just a few (n,m)'s. Nevertheless, the results suggest that much improved chemical separation methods are needed to produce nanotube electronics at a large scale.

  View details for DOI 10.1021/ja7106492

  View details for Web of Science ID 000253400900071

  View details for PubMedID 18251484

• Circulation and long-term fate of functionalized, biocompatible single-walled carbon nanotubes in mice probed by Raman spectroscopy PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Liu, Z., Davis, C., Cai, W., He, L., Chen, X., Dai, H. 2008; 105 (5): 1410-1415

  Abstract

  Carbon nanotubes are promising new materials for molecular delivery in biological systems. The long-term fate of nanotubes intravenously injected into animals in vivo is currently unknown, an issue critical to potential clinical applications of these materials. Here, using the intrinsic Raman spectroscopic signatures of single-walled carbon nanotubes (SWNTs), we measured the blood circulation of intravenously injected SWNTs and detect SWNTs in various organs and tissues of mice ex vivo over a period of three months. Functionalization of SWNTs by branched polyethylene-glycol (PEG) chains was developed, enabling thus far the longest SWNT blood circulation up to 1 day, relatively low uptake in the reticuloendothelial system (RES), and near-complete clearance from the main organs in approximately 2 months. Raman spectroscopy detected SWNT in the intestine, feces, kidney, and bladder of mice, suggesting excretion and clearance of SWNTs from mice via the biliary and renal pathways. No toxic side effect of SWNTs to mice was observed in necropsy, histology, and blood chemistry measurements. These findings pave the way to future biomedical applications of carbon nanotubes.

  View details for DOI 10.1073/pnas.0707654105

  View details for Web of Science ID 000253077900007

  View details for PubMedID 18230737

  View details for PubMedCentralID PMC2234157

• Selective probing and imaging of cells with single walled carbon nanotubes as near-infrared fluorescent molecules NANO LETTERS Welsher, K., Liu, Z., Daranciang, D., Dai, H. 2008; 8 (2): 586-590

  Abstract

  Fluorescent molecules emitting in the near-infrared (NIR, wavelength approximately 0.8-2 microm) are relatively scarce and have been actively sought for biological applications because cells and tissues exhibit little auto-fluorescence in this region. Here, we report the use of semiconducting single-walled carbon nanotubes (SWNTs) as near-infrared fluorescent tags for selective probing of cell surface receptors and cell imaging. Biologically inert SWNTs with polyethyleneglycol functionalization are conjugated to antibodies such as Rituxan to selectively recognize CD20 cell surface receptor on B-cells with little nonspecific binding to negative T-cells and Herceptin to recognize HER2/neu positive breast cancer cells. We image selective SWNT-antibody binding to cells by detecting the intrinsic NIR photoluminescence of nanotubes. We observe ultralow NIR autofluorescence for various cells, an advantageous feature over high autofluorescence and large variations between cells lines in the visible. This establishes SWNTs as novel NIR fluorophors for sensitive and selective biological detections and imaging in vitro and potentially in vivo. Further, our results clearly show that the interactions between carbon nanotubes and living cells are strongly dependent on surface functionalization of nanotubes.

  View details for DOI 10.1021/nl072949q

  View details for Web of Science ID 000253166200039

  View details for PubMedID 18197719

• Hydrogen storage in carbon nanotubes through the formation of stable C-H bonds NANO LETTERS Nikitin, A., Li, X., Zhang, Z., Ogasawara, H., Dai, H., Nilsson, A. 2008; 8 (1): 162-167

  Abstract

  To determine if carbon-based materials can be used for hydrogen storage, we have studied hydrogen chemisorption in single-walled carbon nanotubes. Using atomic hydrogen as the hydrogenation agent, we demonstrated that maximal degree of nanotube hydrogenation depends on the nanotube diameter, and for the diameter values around 2.0 nm nanotube-hydrogen complexes with close to 100% hydrogenation exist and are stable at room temperature. This means that specific carbon nanotubes can have a hydrogen storage capacity of more than 7 wt % through the formation of reversible C-H bonds.

  View details for DOI 10.1021/nl072325k

  View details for Web of Science ID 000252257700029

  View details for PubMedID 18088150

• Nano-Graphene Oxide for Cellular Imaging and Drug Delivery. Nano research Sun, X., Liu, Z., Welsher, K., Robinson, J. T., Goodwin, A., Zaric, S., Dai, H. 2008; 1 (3): 203-212

  Abstract

  Two-dimensional graphene offers interesting electronic, thermal, and mechanical properties that are currently being explored for advanced electronics, membranes, and composites. Here we synthesize and explore the biological applications of nano-graphene oxide (NGO), i.e., single-layer graphene oxide sheets down to a few nanometers in lateral width. We develop functionalization chemistry in order to impart solubility and compatibility of NGO in biological environments. We obtain size separated pegylated NGO sheets that are soluble in buffers and serum without agglomeration. The NGO sheets are found to be photoluminescent in the visible and infrared regions. The intrinsic photoluminescence (PL) of NGO is used for live cell imaging in the near-infrared (NIR) with little background. We found that simple physisorption via pi-stacking can be used for loading doxorubicin, a widely used cancer drug onto NGO functionalized with antibody for selective killing of cancer cells in vitro. Owing to its small size, intrinsic optical properties, large specific surface area, low cost, and useful non-covalent interactions with aromatic drug molecules, NGO is a promising new material for biological and medical applications.

  View details for DOI 10.1007/s12274-008-8021-8

  View details for PubMedID 20216934

  View details for PubMedCentralID PMC2834318

• Carbon nanotube synthesis and organization CARBON NANOTUBES Joselevich, E., Dai, H., Liu, J., Hata, K., Windle, A. H. 2008; 111: 101-164

  View details for Web of Science ID 000253476700005

• Selective synthesis combined with chemical separation of single-walled carbon nanotubes for chirality selection JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Li, X., Tu, X., Zaric, S., Welsher, K., Seo, W. S., Zhao, W., Dai, H. 2007; 129 (51): 15770-?

  Abstract

  Single-walled carbon nanotubes (SWNTs) are potential materials for future nanoelectronics. Since the electronic and optical properties of SWNTs strongly depend on tube diameter and chirality, obtaining SWNTs with narrow (n,m) chirality distribution by selective growth or chemical separation has been an active area of research. Here, we demonstrate that a new, bimetallic FeRu catalyst affords SWNT growth with narrow diameter and chirality distribution in methane CVD. At 600 degrees C, methane CVD on FeRu catalyst produced predominantly (6,5) SWNTs according to UV-vis-NIR absorption and photoluminescence excitation/emission (PLE) spectroscopic characterization. At 850 degrees C, the dominant semiconducting species produced are (8,4), (7,6), and (7,5) SWNTs, with much narrower distributions in diameter and chirality than materials grown by other catalysts. Further, we show that narrow diameter/chirality growth combined with chemical separation by ion exchange chromatography (IEC) greatly facilitates achieving single (m,n) SWNT samples, as demonstrated by obtaining highly enriched (8,4) SWNTs with near elimination of metallic SWNTs existing in the as-grown material.

  View details for DOI 10.1021/ja077886s

  View details for Web of Science ID 000251974000021

  View details for PubMedID 18052285

• Electrically driven light emission from hot single-walled carbon nanotubes at various temperatures and ambient pressures APPLIED PHYSICS LETTERS Wang, X., Zhang, L., Lu, Y., Dai, H., Kato, Y. K., Pop, E. 2007; 91 (26)

  View details for DOI 10.1063/1.2827281

  View details for Web of Science ID 000251987400002

• Moment switching in nanotube magnetic force probes NANOTECHNOLOGY Kirtley, J. R., Deng, Z., Luan, L., Yenilmez, E., Dai, H., Moler, K. A. 2007; 18 (46)

  Abstract

  Magnetic images of high density vertically recorded media using metal-coated carbon nanotube tips exhibit a doubling of the spatial frequency under some conditions (Deng et al 2004 Appl. Phys. Lett. 85 6263). Here we demonstrate that this spatial frequency doubling is due to the switching of the moment direction of the nanotube tip. This results in a signal which is proportional to the absolute value of the signal normally observed in MFM. Our modeling indicates that a significant fraction of the tip volume is involved in the observed switching, and that it should be possible to image high bit densities with nanotube magnetic force sensors.

  View details for DOI 10.1088/0957-4484/18/46/465506

  View details for Web of Science ID 000250200600013

  View details for PubMedID 21730480

• Theoretical investigations on thermal light emission from metallic carbon nanotubes IEEE TRANSACTIONS ON NANOTECHNOLOGY Ouyang, Y., Mann, D., Dai, H., Guo, J. 2007; 6 (6): 682-687

  View details for DOI 10.1109/TNANO.2007.907253

  View details for Web of Science ID 000251032300013

• Supramolecular chemistry on water-soluble carbon nanotubes for drug loading and delivery ACS NANO Liu, Z., Sun, X., Nakayama-Ratchford, N., Dai, H. 2007; 1 (1): 50-56

  Abstract

  We show that large surface areas exist for supramolecular chemistry on single-walled carbon nanotubes (SWNTs) prefunctionalized noncovalently or covalently by common surfactant or acid-oxidation routes. Water-soluble SWNTs with poly(ethylene glycol) (PEG) functionalization via these routes allow for surprisingly high degrees of pi-stacking of aromatic molecules, including a cancer drug (doxorubicin) with ultrahigh loading capacity, a widely used fluorescence molecule (fluorescein), and combinations of molecules. Binding of molecules to nanotubes and their release can be controlled by varying the pH. The strength of pi-stacking of aromatic molecules is dependent on nanotube diameter, leading to a method for controlling the release rate of molecules from SWNTs by using nanotube materials with suitable diameter. This work introduces the concept of "functionalization partitioning" of SWNTs, i.e., imparting multiple chemical species, such as PEG, drugs, and fluorescent tags, with different functionalities onto the surface of the same nanotube. Such chemical partitioning should open up new opportunities in chemical, biological, and medical applications of novel nanomaterials.

  View details for DOI 10.1021/nn700040t

  View details for Web of Science ID 000252012200011

  View details for PubMedID 19203129

• Tomonaga-luttinger liquid features in ballistic single-walled carbon nanotubes: Conductance and shot noise PHYSICAL REVIEW LETTERS Kim, N. Y., Recher, P., Oliver, W. D., Yamamoto, Y., Kong, J., Dai, H. 2007; 99 (3)

  Abstract

  We study the electrical transport properties of well-contacted ballistic single-walled carbon nanotubes in a three-terminal configuration at low temperatures. We observe signatures of strong electron-electron interactions: the conductance exhibits bias-voltage-dependent amplitudes of quantum interference oscillation, and both the current noise and Fano factor manifest bias-voltage-dependent power-law scalings. We analyze our data within the Tomonaga-Luttinger liquid model using the nonequilibrium Keldysh formalism and find qualitative and quantitative agreement between experiment and theory.

  View details for DOI 10.1103/PhyRevLett.99.036802

  View details for Web of Science ID 000248194700038

  View details for PubMedID 17678308

• Soluble single-walled carbon nanotubes as longboat delivery systems for Platinum(IV) anticancer drug design JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Feazell, R. P., Nakayama-Ratchford, N., Dai, H., Lippard, S. J. 2007; 129 (27): 8438-?

  View details for DOI 10.1021/ja073231f

  View details for Web of Science ID 000247759400020

  View details for PubMedID 17569542

  View details for PubMedCentralID PMC2505197

• Measuring the capacitance of individual semiconductor nanowires for carrier mobility assessment NANO LETTERS Tu, R., Zhang, L., Nishi, Y., Dai, H. 2007; 7 (6): 1561-1565

  Abstract

  Capacitance-voltage characteristics of individual germanium nanowire field effect transistors were directly measured and used to assess carrier mobility in nanowires for the first time, thereby removing uncertainties in calculated mobility due to device geometries, surface and interface states, and gate dielectric constants and thicknesses. Direct experimental evidence showed that surround-gated nanowire transistors exhibit higher capacitance and better electrostatic gate control than top-gated devices, and are the most promising structure for future high performance nanoelectronics.

  View details for DOI 10.1021/nl070378w

  View details for Web of Science ID 000247186800023

  View details for PubMedID 17488051

• Electrical and thermal transport in metallic single-wall carbon nanotubes on insulating substrates JOURNAL OF APPLIED PHYSICS Pop, E., Mann, D. A., Goodson, K. E., Dai, H. 2007; 101 (9)

  View details for DOI 10.1063/1.2717855

  View details for Web of Science ID 000246567900049

• Langmuir-Blodgett assembly of densely aligned single-walled carbon nanotubes from bulk materials JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Li, X., Zhang, L., Wang, X., Shimoyama, I., Sun, X., Seo, W., Dai, H. 2007; 129 (16): 4890-?

  View details for DOI 10.1021/ja071114e

  View details for Web of Science ID 000245782800017

  View details for PubMedID 17394327

• Noncovalent functionalization of carbon nanotubes by fluorescein-polyethylene glycol: Supramolecular conjugates with pH-dependent absorbance and fluorescence JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Nakayama-Ratchford, N., Bangsaruntip, S., Sun, X., Welsher, K., Dai, H. 2007; 129 (9): 2448-?

  View details for DOI 10.1021/ja068684j

  View details for Web of Science ID 000244731300020

  View details for PubMedID 17284037

• siRNA delivery into human T cells and primary cells with carbon-nanotube transporters ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Liu, Z., Winters, M., Holodniy, M., Dai, H. 2007; 46 (12): 2023-2027

  View details for DOI 10.1002/anie.200604295

  View details for Web of Science ID 000245071000016

  View details for PubMedID 17290476

• Electrically driven thermal light emission from individual single-walled carbon nanotubes NATURE NANOTECHNOLOGY Mann, D., Kato, Y. K., Kinkhabwala, A., Pop, E., Cao, J., Wang, X., Zhang, L., Wang, Q., Guo, J., Dai, H. 2007; 2 (1): 33-38

  View details for DOI 10.1038/nnano.2006.169

  View details for Web of Science ID 000243902900012

  View details for PubMedID 18654204

• In vivo biodistribution and highly efficient tumour targeting of carbon nanotubes in mice NATURE NANOTECHNOLOGY Liu, Z., Cai, W., He, L., Nakayama, N., Chen, K., Sun, X., Chen, X., Dai, H. 2007; 2 (1): 47-52

  View details for DOI 10.1038/nnano.2006.170

  View details for Web of Science ID 000243902900015

  View details for PubMedID 18654207

• Parallel core-shell metal-dielectric-semiconductor germanium nanowires for high-current surround-gate field-effect transistors NANO LETTERS Zhang, L., Tu, R., Dai, H. 2006; 6 (12): 2785-2789

  Abstract

  Core-shell germanium nanowires (GeNW) are formed with a single-crystalline Ge core and concentric shells of nitride and silicon passivation layer by chemical vapor deposition (CVD), an Al2O3 gate dielectric layer by atomic layer deposition (ALD), and an Al metal surround-gate (SG) shell by isotropic magnetron sputter deposition. Surround-gate nanowire field-effect transistors (FETs) are then constructed using a novel self-aligned fabrication approach. Individual SG GeNW FETs show improved switching over GeNW FETs with planar gate stacks owing to improved electrostatics. FET devices comprised of multiple quasi-aligned SG GeNWs in parallel are also constructed. Collectively, tens of SG GeNWs afford on-currents exceeding 0.1 mA at low source-drain bias voltages. The self-aligned surround-gate scheme can be generalized to various semiconductor nanowire materials.

  View details for DOI 10.1021/nl061833b

  View details for Web of Science ID 000242786500027

  View details for PubMedID 17163706

• FeCo/graphitic-shell nanocrystals as advanced magnetic-resonance-imaging and near-infrared agents NATURE MATERIALS Seo, W. S., Lee, J. H., Sun, X., Suzuki, Y., Mann, D., Liu, Z., Terashima, M., Yang, P. C., McConnell, M. V., Nishimura, D. G., Dai, H. 2006; 5 (12): 971-976

  Abstract

  Nanocrystals with advanced magnetic or optical properties have been actively pursued for potential biological applications, including integrated imaging, diagnosis and therapy. Among various magnetic nanocrystals, FeCo has superior magnetic properties, but it has yet to be explored owing to the problems of easy oxidation and potential toxicity. Previously, FeCo nanocrystals with multilayered graphitic carbon, pyrolytic carbon or inert metals have been obtained, but not in the single-shelled, discrete, chemically functionalized and water-soluble forms desired for biological applications. Here, we present a scalable chemical vapour deposition method to synthesize FeCo/single-graphitic-shell nanocrystals that are soluble and stable in water solutions. We explore the multiple functionalities of these core-shell materials by characterizing the magnetic properties of the FeCo core and near-infrared optical absorbance of the single-layered graphitic shell. The nanocrystals exhibit ultra-high saturation magnetization, r1 and r2 relaxivities and high optical absorbance in the near-infrared region. Mesenchymal stem cells are able to internalize these nanoparticles, showing high negative-contrast enhancement in magnetic-resonance imaging (MRI). Preliminary in vivo experiments achieve long-lasting positive-contrast enhancement for vascular MRI in rabbits. These results point to the potential of using these nanocrystals for integrated diagnosis and therapeutic (photothermal-ablation) applications.

  View details for DOI 10.1038/nmat1775

  View details for PubMedID 17115025

• Selective etching of metallic carbon nanotubes by gas-phase reaction SCIENCE Zhang, G., Qi, P., Wang, X., Lu, Y., Li, X., Tu, R., Bangsaruntip, S., Mann, D., Zhang, L., Dai, H. 2006; 314 (5801): 974-977

  Abstract

  Metallic and semiconducting carbon nanotubes generally coexist in as-grown materials. We present a gas-phase plasma hydrocarbonation reaction to selectively etch and gasify metallic nanotubes, retaining the semiconducting nanotubes in near-pristine form. With this process, 100% of purely semiconducting nanotubes were obtained and connected in parallel for high-current transistors. The diameter- and metallicity-dependent "dry" chemical etching approach is scalable and compatible with existing semiconductor processing for future integrated circuits.

  View details for DOI 10.1126/science.1133781

  View details for Web of Science ID 000241896000047

  View details for PubMedID 17095698

• Germanium nanowires: from synthesis, surface chemistry, and assembly to devices APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING Wang, D., Dai, H. 2006; 85 (3): 217-225

  View details for DOI 10.1007/s00339-006-3704-z

  View details for Web of Science ID 000241354900002

• Single walled carbon nanotubes for transport and delivery of biological cargos 20th International Winterschool/Euroconference on Electronic Properties of Novel Materials Kam, N. W., Dai, H. WILEY-V C H VERLAG GMBH. 2006: 3561–66

  View details for DOI 10.1002/pssb.200669226

  View details for Web of Science ID 000242187000125

• Neural stimulation with a carbon nanotube microelectrode array NANO LETTERS Wang, K., Fishman, H. A., Dai, H., Harris, J. S. 2006; 6 (9): 2043-2048

  Abstract

  We present a novel prototype neural interface using vertically aligned multiwalled carbon nanotube (CNT) pillars as microelectrodes. Functionalized hydrophilic CNT microelectrodes offer a high charge injection limit (1-1.6 mC/cm2) without faradic reactions. The first repeated in vitro stimulation of hippocampal neurons with CNT electrodes is demonstrated. These results suggest that CNTs are capable of providing far safer and more efficacious solutions for neural prostheses than previous metal electrode approaches.

  View details for DOI 10.1021/nl061241t

  View details for Web of Science ID 000240465100037

  View details for PubMedID 16968023

• FUEL 239-Hydrogen storage enhancement of HiPCO SWNTs by palladium catalyst doping Lee, Y., Bhowmick, R., Dai, H., Clemens, B. M. AMER CHEMICAL SOC. 2006

  View details for Web of Science ID 000207781605094

• Electrical transport properties and field effect transistors of carbon nanotubes NANO Dai, H., Javey, A., Pop, E., Mann, D., Kim, W., Lu, Y. 2006; 1 (1): 1-13

  View details for Web of Science ID 000202998500001

• Hydrogenation and hydrocarbonation and etching of single-walled carbon nanotubes JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Zhang, G., Qi, P., Wang, X., Lu, Y., Mann, D., Li, X., Dai, H. 2006; 128 (18): 6026-6027

  Abstract

  We present a systematic experimental investigation of the reactions between hydrogen plasma and single-walled carbon nanotubes (SWNTs) at various temperatures. Microscopy, infrared (IR) and Raman spectroscopy, and electrical transport measurements are carried out to investigate the properties of SWNTs after hydrogenation. Structural deformations, drastically reduced electrical conductance, and an increased semiconducting nature of SWNTs upon sidewall hydrogenation are observed. These changes are reversible upon thermal annealing at 500 degrees C via dehydrogenation. Harsh plasma or high temperature reactions lead to etching of nanotubes likely via hydrocarbonation. Smaller SWNTs are markedly less stable against hydrocarbonation than larger tubes. The results are fundamental and may have implications to basic and practical applications including hydrogen storage, sensing, band gap engineering for novel electronics, and new methods of manipulation, functionalization, and etching of nanotubes.

  View details for DOI 10.1021/ja061324b

  View details for Web of Science ID 000237468900022

  View details for PubMedID 16669658

• DNA functionalization of carbon nanotubes for ultrathin atomic layer deposition of high kappa dielectrics for nanotube transistors with 60 mV/decade switching JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Lu, Y. R., Bangsaruntip, S., Wang, X. R., Zhang, L., Nishi, Y., Dai, H. J. 2006; 128 (11): 3518-3519

  Abstract

  For single-walled carbon nanotube (SWNT) field effect transistors, vertical scaling of high kappa dielectrics by atomic layer deposition (ALD) currently stands at approximately 8 nm with a subthreshold swing S approximately 70-90 mV/decade at room temperature. ALD on as-grown pristine SWNTs is incapable of producing a uniform and conformal dielectric layer due to the lack of functional groups on nanotubes and because nucleation of an oxide dielectric layer in the ALD process hinges upon covalent chemisorption on reactive groups on surfaces. Here, we show that by noncovalent functionalization of SWNTs with poly-T DNA molecules (dT40-DNA), one can impart functional groups of sufficient density and stability for uniform and conformal ALD of high kappa dielectrics on SWNTs with thickness down to 2-3 nm. This enables approaching the ultimate vertical scaling limit of nanotube FETs and reliably achieving S approximately 60 mV/decade at room temperature, and S approximately 50 mV/decade in the band-to-band tunneling regime of ambipolar transport. We have also carried out microscopy investigations to understand ALD processes on SWNTs with and without DNA functionalization.

  View details for DOI 10.1021/ja058836v

  View details for Web of Science ID 000236299700024

  View details for PubMedID 16536515

• Nanotube manipulation with focused ion beam APPLIED PHYSICS LETTERS Deng, Z. F., Yenilmez, E., Reilein, A., Leu, J., DAI, H. J., Moler, K. A. 2006; 88 (2)

  View details for DOI 10.1063/1.2161395

  View details for Web of Science ID 000234606900073

• Thermal conductance of an individual single-wall carbon nanotube above room temperature NANO LETTERS Pop, E., Mann, D., Wang, Q., Goodson, K. E., Dai, H. J. 2006; 6 (1): 96-100

  Abstract

  The thermal properties of a suspended metallic single-wall carbon nanotube (SWNT) are extracted from its high-bias (I-V) electrical characteristics over the 300-800 K temperature range, achieved by Joule self-heating. The thermal conductance is approximately 2.4 nW/K, and the thermal conductivity is nearly 3500 Wm(-1)K(-1) at room temperature for a SWNT of length 2.6 mum and diameter 1.7 nm. A subtle decrease in thermal conductivity steeper than 1/T is observed at the upper end of the temperature range, which is attributed to second-order three-phonon scattering between two acoustic modes and one optical mode. We discuss sources of uncertainty and propose a simple analytical model for the SWNT thermal conductivity including length and temperature dependence.

  View details for DOI 10.1021/nl052145f

  View details for Web of Science ID 000235532400018

  View details for PubMedID 16402794

• Electro-thermal transport in silicon and carbon nanotube devices 14th International Conference on Nonequilibrium Carrier Dynamics in Semiconductors Pop, E., Mann, D., ROWLETTE, J., Goodson, K., Dai, H. SPRINGER-VERLAG BERLIN. 2006: 195–199

  View details for Web of Science ID 000242486900044

• Thermal properties of metal-coated vertically-aligned single wall nanotube films 10th Intersociety Conference on Thermal and Thermomechanical Phenomena in Electronic Systems Panzer, M., Zhang, G., Mann, D., Hu, X., Pop, E., Dai, H., Goodson, K. E. IEEE. 2006: 1306–1313

  View details for Web of Science ID 000243624500180

• Carbon nanotubes: From growth, placement and assembly control to 60mV/decade and sub-60 mV/decade tunnel transistors IEEE International Electron Devices Meeting Zhang, G., Wang, X., Li, X., Lu, Y., Javey, A., Dai, H. IEEE. 2006: 160–163

  View details for Web of Science ID 000247357700042

• Carbon nanotubes as intracellular transporters for proteins and DNA: An investigation of the uptake mechanism and pathway ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Kam, N. W., Liu, Z. A., Dai, H. J. 2006; 45 (4): 577-581

  View details for DOI 10.1002/anie.200503389

  View details for Web of Science ID 000234769200008

  View details for PubMedID 16345107

• Hydrogenation of single-walled carbon nanotubes PHYSICAL REVIEW LETTERS Nikitin, A., Ogasawara, H., Mann, D., Denecke, R., Zhang, Z., Dai, H., Cho, K., Nilsson, A. 2005; 95 (22)

  Abstract

  Towards the development of a useful mechanism for hydrogen storage, we have studied the hydrogenation of single-walled carbon nanotubes with atomic hydrogen using core-level photoelectron spectroscopy and x-ray absorption spectroscopy. We find that atomic hydrogen creates C-H bonds with the carbon atoms in the nanotube walls, and such C-H bonds can be completely broken by heating to 600 degrees C. We demonstrate approximately 65 +/- 15 at % hydrogenation of carbon atoms in the single-walled carbon nanotubes, which is equivalent to 5.1 +/- 1.2 wt % hydrogen capacity. We also show that the hydrogenation is a reversible process.

  View details for DOI 10.1103/PhysRevLett.95.225507

  View details for Web of Science ID 000233458500040

  View details for PubMedID 16384236

• Ultra-high-yield growth of vertical single-walled carbon nanotubes: Hidden roles of hydrogen and oxygen PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Zhang, G. Y., Mann, D., Zhang, L., Javey, A., Li, Y. M., Yenilmez, E., Wang, Q., McVittie, J. P., Nishi, Y., Gibbons, J., Dai, H. J. 2005; 102 (45): 16141-16145

  Abstract

  An oxygen-assisted hydrocarbon chemical vapor deposition method is developed to afford large-scale, highly reproducible, ultra-high-yield growth of vertical single-walled carbon nanotubes (V-SWNTs). It is revealed that reactive hydrogen species, inevitable in hydrocarbon-based growth, are damaging to the formation of sp(2)-like SWNTs in a diameter-dependent manner. The addition of oxygen scavenges H species and provides a powerful control over the C/H ratio to favor SWNT growth. The revelation of the roles played by hydrogen and oxygen leads to a unified and universal optimum-growth condition for SWNTs. Further, a versatile method is developed to form V-SWNT films on any substrate, lifting a major substrate-type limitation for aligned SWNTs.

  View details for DOI 10.1073/pnas.0507064102

  View details for PubMedID 16263931

• Electrical contacts to carbon nanotubes down to 1 nm in diameter APPLIED PHYSICS LETTERS Kim, W., Javey, A., Tu, R., Cao, J., Wang, Q., Dai, H. J. 2005; 87 (17)

  View details for DOI 10.1063/1.2108127

  View details for Web of Science ID 000232723700050

• Negative differential conductance and hot phonons in suspended nanotube molecular wires PHYSICAL REVIEW LETTERS Pop, E., Mann, D., Cao, J., Wang, Q., Goodson, K. E., Dai, H. J. 2005; 95 (15)

  Abstract

  Freely suspended metallic single-walled carbon nanotubes (SWNTs) exhibit reduced current carrying ability compared to those lying on substrates, and striking negative differential conductance at low electric fields. Theoretical analysis reveals significant self-heating effects including electron scattering by hot nonequilibrium optical phonons. Electron transport characteristics under strong self-heating are exploited for the first time to probe the thermal conductivity of individual SWNTs (approximately 3600 W m-1 K-1 at T=300 K) up to approximately 700 K, and reveal a 1/T dependence expected for umklapp phonon scattering at high temperatures.

  View details for DOI 10.1103/PhysRevLett.95.155505

  View details for Web of Science ID 000232443400039

  View details for PubMedID 16241738

• Electron transport in very clean, as-grown suspended carbon nanotubes NATURE MATERIALS Cao, J., Wang, Q., Dai, H. 2005; 4 (10): 745-749

  Abstract

  Single-walled carbon nanotubes have shown a wealth of quantum transport phenomena thus far. Defect-free, unperturbed single-walled carbon nanotubes with well behaved or tunable metal contacts are important for probing the intrinsic electrical properties of nanotubes. Meeting these conditions experimentally is non-trivial owing to numerous disorder and randomizing factors. Here we show that approximately 1-microm-long fully suspended single-walled carbon nanotubes grown in place between metal contacts afford devices with well defined characteristics over much wider energy ranges than nanotubes pinned on substrates. Various low-temperature transport regimes in true-metallic, small- and large-bandgap semiconducting nanotubes are observed, including quantum states shell-filling, -splitting and -crossing in magnetic fields owing to the Aharonov-Bohm effect. The clean transport data show a correlation between the contact junction resistance and the various transport regimes in single-walled-carbon-nanotube devices. Furthermore, we show that electrical transport data can be used to probe the band structures of nanotubes, including nonlinear band dispersion.

  View details for DOI 10.1038/nmat1478

  View details for Web of Science ID 000232229500012

  View details for PubMedID 16142240

• Functionalization of carbon nanotubes via cleavable disulfide bonds for efficient intracellular delivery of siRNA and potent gene silencing JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Kam, N. W., Liu, Z., Dai, H. J. 2005; 127 (36): 12492-12493

  Abstract

  We present a novel functionalization scheme for single-walled carbon nanotubes (SWNTs) to afford nanotube-biomolecule conjugates with the incorporation of cleavable bonds to enable controlled molecular releasing from nanotube surfaces, thus creating "smart" nanomaterials with high potential for chemical and biological applications. With this versatile functionalization, we demonstrate transporting, enzymatic cleaving and releasing of DNA from SWNT transporters, and subsequent nuclear translocation of DNA oligonucleotides in mammalian cells. We further show highly efficient delivery of siRNA by SWNTs and achieving more potent RNAi functionality than a widely used conventional transfection agent. Thus, the novel functionalization of SWNTs with cleavable bonds is highly promising for a wide range of applications including gene and protein therapy.

  View details for DOI 10.1021/ja053962k

  View details for Web of Science ID 000232039100030

  View details for PubMedID 16144388

• Regular arrays of 2 nm metal nanoparticles for deterministic synthesis of nanomaterials JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Javey, A., Dai, H. J. 2005; 127 (34): 11942-11943

  Abstract

  A novel method is developed to enable the formation, positioning, and patterning of individual metal nanoclusters with controllable and monodispersed sizes down to 1-2 nm scale. The method is generic for fabricating designed arrays of virtually any type of metal nanoparticles well below 10 nm. Among the wide range of potential applications in surface and materials science, the nanoparticle arrays are used for deterministic synthesis of monodispersed single-walled carbon nanotubes at individually controlled locations with near 1:1 yield, reaching one of the ultimate goals of nanotube synthesis.

  View details for DOI 10.1021/ja0536668

  View details for Web of Science ID 000231605900032

  View details for PubMedID 16117524

• Oxidation resistant germanium nanowires: Bulk synthesis, long chain alkanethiol functionalization, and Langmuir-Blodgett assembly JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Wang, D. W., Chang, Y. L., Liu, Z., Dai, H. J. 2005; 127 (33): 11871-11875

  Abstract

  A simple method is developed to synthesize gram quantities of uniform Ge nanowires (GeNWs) by chemical vapor deposition on preformed, monodispersed seed particles loaded onto a high surface area silica support. Various chemical functionalization schemes are investigated to passivate the GeNW surfaces using alkanethiols and alkyl Grignard reactions. The stability of functionalization against oxidation of germanium for various alkyl chain lengths is elucidated by X-ray photoelectron spectroscopy. Among all schemes tested, long chain alkanethiols (> or = C12) are found to impart the most stable GeNW passivation against oxidation upon extended exposure to ambient air. Further, the chemically functionalized oxidation-resistant nanowires are soluble in organic solvents and can be readily assembled into close-packed Langmuir-Blodgett films potentially useful for future high performance electronic devices.

  View details for DOI 10.1021/ja053836g

  View details for Web of Science ID 000231454100074

  View details for PubMedID 16104766

• Carbon nanotubes as multifunctional biological transporters and near-infrared agents for selective cancer cell destruction PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Kam, N. W., O'Connell, M., Wisdom, J. A., Dai, H. J. 2005; 102 (33): 11600-11605

  Abstract

  Biological systems are known to be highly transparent to 700- to 1,100-nm near-infrared (NIR) light. It is shown here that the strong optical absorbance of single-walled carbon nanotubes (SWNTs) in this special spectral window, an intrinsic property of SWNTs, can be used for optical stimulation of nanotubes inside living cells to afford multifunctional nanotube biological transporters. For oligonucleotides transported inside living cells by nanotubes, the oligos can translocate into cell nucleus upon endosomal rupture triggered by NIR laser pulses. Continuous NIR radiation can cause cell death because of excessive local heating of SWNT in vitro. Selective cancer cell destruction can be achieved by functionalization of SWNT with a folate moiety, selective internalization of SWNTs inside cells labeled with folate receptor tumor markers, and NIR-triggered cell death, without harming receptor-free normal cells. Thus, the transporting capabilities of carbon nanotubes combined with suitable functionalization chemistry and their intrinsic optical properties can lead to new classes of novel nanomaterials for drug delivery and cancer therapy.

  View details for DOI 10.1073/pnas.0502680102

  View details for Web of Science ID 000231317000008

  View details for PubMedID 16087878

  View details for PubMedCentralID PMC1187972

• Carbon nanotubes as intracellular protein transporters: Generality and biological functionality JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Kam, N. W., Dai, H. J. 2005; 127 (16): 6021-6026

  Abstract

  Various proteins adsorb spontaneously on the sidewalls of acid-oxidized single-walled carbon nanotubes. This simple nonspecific binding scheme can be used to afford noncovalent protein-nanotube conjugates. The proteins are found to be readily transported inside various mammalian cells with nanotubes acting as the transporter via the endocytosis pathway. Once released from the endosomes, the internalized protein-nanotube conjugates can enter into the cytoplasm of cells and perform biological functions, evidenced by apoptosis induction by transported cytochrome c. Carbon nanotubes represent a new class of molecular transporters potentially useful for future in vitro and in vivo protein delivery applications.

  View details for DOI 10.1021/ja050062v

  View details for Web of Science ID 000228602600065

  View details for PubMedID 15839702

• Carbon nanotubes: Synthesis, properties and new directions (tutorial). 229th National Meeting of the American-Chemical-Society (ACS) Dai, H. J. AMER CHEMICAL SOC. 2005: U910–U910

  View details for Web of Science ID 000235066604027

• Robustness, scalability, and integration of a wound-response gene expression signature in predicting breast cancer survival PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Chang, H. Y., Nuyten, D. S., Sneddon, J. B., Hastie, T., Tibshirani, R., Sorlie, T., Dai, H. Y., He, Y. D., Van't Veer, L. J., Bartelink, H., van de Rijn, M., Brown, P. O., van de Vijver, M. J. 2005; 102 (10): 3738-3743

  Abstract

  Based on the hypothesis that features of the molecular program of normal wound healing might play an important role in cancer metastasis, we previously identified consistent features in the transcriptional response of normal fibroblasts to serum, and used this "wound-response signature" to reveal links between wound healing and cancer progression in a variety of common epithelial tumors. Here, in a consecutive series of 295 early breast cancer patients, we show that both overall survival and distant metastasis-free survival are markedly diminished in patients whose tumors expressed this wound-response signature compared to tumors that did not express this signature. A gene expression centroid of the wound-response signature provides a basis for prospectively assigning a prognostic score that can be scaled to suit different clinical purposes. The wound-response signature improves risk stratification independently of known clinico-pathologic risk factors and previously established prognostic signatures based on unsupervised hierarchical clustering ("molecular subtypes") or supervised predictors of metastasis ("70-gene prognosis signature").

  View details for DOI 10.1073/pnas.0409462102

  View details for PubMedID 15701700

• Piezoresistance of carbon nanotubes on deformable thin-film membranes APPLIED PHYSICS LETTERS Grow, R. J., Wang, Q., Cao, J., Wang, D. W., Dai, H. J. 2005; 86 (9)

  View details for DOI 10.1063/1.1872221

  View details for Web of Science ID 000228991600055

• Resonances in J/psi -> phi pi(+)pi(-) and phi K+K- PHYSICS LETTERS B Ablikim, M., Bai, J. Z., Ban, Y., Bian, J. G., Bugg, D., Cai, X., Chang, J. F., Chen, H. F., Chen, H. S., Chen, H. X., Chen, J. C., Chen, J., Chen, J., CHEN, M. L., Chen, Y. B., Chi, S. P., Chu, Y. P., Cui, X. Z., Dai, H. L., Dai, Y. S., Deng, Z. Y., Dong, L. Y., Dong, Q. F., Du, S. X., Du, Z. Z., Fang, J., Fang, S. S., Fu, C. D., Fu, H. Y., Gao, C. S., Gao, Y. N., Gong, M. Y., Gong, W. X., Gu, S. D., Guo, Y., Guo, Y. Q., Guo, Z. J., Harris, F. A., He, K. L., He, M., He, X., Heng, Y. K., Hu, H. M., Hu, T., Huang, G. S., Huang, X. P., Huang, X. T., Ji, X. B., Jiang, C. H., Jiang, X. S., Jin, D. P., Jin, S., Jin, Y., Jin, Y., Lai, Y. F., Li, F., Li, G., Li, H. H., Li, J., Li, J. C., Li, Q. J., Li, R. Y., Li, S. M., Li, W. D., Li, W. G., Li, X. L., Li, X. Q., Li, Y. L., Liang, Y. F., Liao, H. B., Liu, C. X., Liu, F., Liu, F., Liu, H. H., Liu, H. M., Liu, J., Liu, J. B., Liu, J. P., Liu, R. G., Liu, Z. A., Liu, Z. X., Lu, F., Lu, G. R., Lu, H. J., Lu, J. G., Luo, C. L., Luo, L. X., Luo, X. L., Ma, F. C., Ma, H. L., Ma, J. M., Ma, L. L., Ma, Q. M., Mae, X. B., Ma, X. Y., Mao, Z. P., Mo, X. H., Nie, J., Nie, Z. D., Olsen, S. L., Peng, H. P., Qi, N. D., Qian, C. D., Qin, H., Qiu, J. F., Ren, Z. Y., Rong, G., Shan, L. Y., Shang, L., Shen, D. L., Shen, X. Y., Sheng, H. Y., Shi, F., Shi, X., Sun, H. S., Sun, J. F., Sun, S. S., Sun, Y. Z., Sun, Z. J., Tang, X., Tao, N., Tian, Y. R., Tong, G. L., Varner, G. S., Wang, D. Y., Wang, J. Z., Wang, K., Wang, L., Wang, L. S., Wang, M., Wang, P., Wang, P. L., Wang, S. Z., Wang, W. F., Wang, Y. F., Wang, Z., Wang, Z. Y., Wang, Z., Zheng, Z., Wei, C. L., Wei, D. H., Wu, Y. M., Xia, X. M., Xie, X. X., Xin, B., Xu, G. F., Xu, H., Xue, S. T., Yan, M. L., Yang, F., Yang, H. X., Yang, J., Yang, Y. X., Ye, M., Ye, M. H., Ye, Y. X., Yi, L. H., Yi, Z. Y., Yu, C. S., Yu, G. W., Yuan, C. Z., Yuan, J. M., Zang, S. L., Zeng, Y., Zeng, Y., Zhang, B. X., Zhang, B. Y., Zhang, C. C., Zhang, D. H., Zhang, H. Y., Zhang, J., Zhang, J. W., Zhang, J. Y., Zhang, Q. J., Zhang, S. Q., Zhang, X. M., Zhang, X. Y., Zhang, Y. Y., Zhang, Y. Y., Zhang, Z. P., Zhang, Z. Q., Zhao, D. X., Zhao, J. B., Zhao, J. W., Zhao, M. G., Zhao, P. P., Zhao, W. R., Zhao, X. J., Zhao, Y. B., Zhao, Z. G., Zheng, H. Q., Zheng, J. P., Zheng, L. S., Zheng, Z. P., Zhong, X. C., Zhou, B. Q., Zhou, G. M., Zhou, L., Zhou, N. F., Zhu, K. J., Zhu, Q. M., Zhu, Y. C., Zhou, Y. S., Zhu, Y. C., Zhu, Z. A., Zhuang, B. A., Zhuang, X. A., Zou, B. S. 2005; 607 (3-4): 243-253

  View details for DOI 10.1016/j.physletb.2004.12.041

  View details for Web of Science ID 000226930000006

• Measurement of ionizing radiation using carbon nanotube field effect transistor PHYSICS IN MEDICINE AND BIOLOGY Tang, X. W., Yang, Y., Kim, W., Wang, Q., Qi, P. F., Dai, H. J., Xing, L. 2005; 50 (3): N23-N31

  Abstract

  Single-walled carbon nanotubes (SWNTs) are a new class of highly promising nanomaterials for future nano-electronics. Here, we present an initial investigation of the feasibility of using SWNT field effect transistors (SWNT-FETs) formed on silicon-oxide substrates and suspended FETs for radiation dosimetry applications. Electrical measurements and atomic force microscopy (AFM) revealed the intactness of SWNT-FET devices after exposure to over 1 Gy of 6 MV therapeutic x-rays. The sensitivity of SWNT-FET devices to x-ray irradiation is elucidated by real-time dose monitoring experiments and accumulated dose reading based on threshold voltage shift. SWNT-FET devices exhibit sensitivities to x-rays that are at least comparable to or orders of magnitude higher than commercial MOSFET (metal-oxide semiconductor field effect transistor) dosimeters and could find applications as miniature dosimeters for microbeam profiling and implantation.

  View details for DOI 10.1088/0031-9155/50/3/N02

  View details for PubMedID 15773731

• High performance n-type carbon nanotube field-effect transistors with chemically doped contacts NANO LETTERS Javey, A., Tu, R., Farmer, D. B., Guo, J., Gordon, R. G., Dai, H. J. 2005; 5 (2): 345-348

  Abstract

  Short channel ( approximately 80 nm) n-type single-walled carbon nanotube (SWNT) field-effect transistors (FETs) with potassium (K) doped source and drain regions and high-kappa gate dielectrics (ALD HfO(2)) are obtained. For nanotubes with diameter approximately 1.6 nm and band gap approximately 0.55 eV, we obtain n-MOSFET-like devices exhibiting high on-currents due to chemically suppressed Schottky barriers at the contacts, subthreshold swing of 70 mV/decade, negligible ambipolar conduction, and high on/off ratios up to 10(6) at a bias voltage of 0.5 V. The results compare favorably with the state-of-the-art silicon n-MOSFETs and demonstrate the potential of SWNTs for future complementary electronics. The effects of doping level on the electrical characteristics of the nanotube devices are discussed.

  View details for DOI 10.1021/nl047931j

  View details for Web of Science ID 000227100500028

  View details for PubMedID 15794623

• Suspended carbon nanotube quantum wires with two gates SMALL Cao, H., Wang, Q., Wang, D. W., Dai, H. J. 2005; 1 (1): 138-141

  Abstract

  Suspended single-walled carbon nanotube devices comprised of high-quality electrical contacts and two electrostatic gates per device have been prepared. Compared to nanotubes pinned on substrates, the suspended devices exhibit little hysteresis related to environmental factors and act as cleaner Fabry-Perot interferometers or single-electron transistors. The high-field saturation currents in the suspended nanotubes related to optical phonon or zone-boundary phonon scattering are significantly lower due to the lack of efficient heat sinking. The multiple-gate design may also facilitate future investigations into the electromechanical properties of nanotube quantum systems.

  View details for DOI 10.1002/smll.200400015

  View details for Web of Science ID 000229117700021

  View details for PubMedID 17193364

• Carbon nanotube electronics 19TH INTERNATIONAL CONFERENCE ON VLSI DESIGN, PROCEEDINGS Javey, A., DAI, H. J. 2005: 453-458

  View details for Web of Science ID 000236463500083

• Fabrication of a carbon nanotube protruding electrode array for a retinal prosthesis Conference on Microfludics, BioMEMS, and Medical Microsystems III Wang, K., Dai, H., Fishman, H. A., Harris, J. S. SPIE-INT SOC OPTICAL ENGINEERING. 2005: 22–29

  View details for DOI 10.1117/12.591153

  View details for Web of Science ID 000228863400006

• Self-aligned 40 nm channel carbon nanotube field-effect transistors with subthreshold swings down to 70mV/decade Conference on Quantum Sensing and Nanophotonic Devices II Javey, A., Farmer, D., Gordon, R., DAI, H. J. SPIE-INT SOC OPTICAL ENGINEERING. 2005: 14–18

  View details for DOI 10.1117/12.584212

  View details for Web of Science ID 000229036500002

• 2,4-dinitrobenzenesulfonyl fluoresceins as fluorescent alternatives to Ellman's reagent in thiol-quantification enzyme assays ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Maeda, H., Matsuno, H., Ushida, M., Katayama, K., Saeki, K., Itoh, N. 2005; 44 (19): 2922-2925

  View details for DOI 10.1002/anie.200500114

  View details for Web of Science ID 000229091300018

  View details for PubMedID 15818626

• Electro-thermal transport in metallic single-wall carbon nanotubes for interconnect applications IEEE International Electron Devices Meeting Pop, E., Mann, D., Reifenberg, J., Goodson, K., Dai, H. J. IEEE. 2005: 261–264

  View details for Web of Science ID 000236225100058

• Deterministic one-to-one synthesis of germanium nanowires and individual gold nanoseed patterning for aligned arrays ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Wang, D. W., Tu, R., Zhang, L., Dai, H. J. 2005; 44 (19): 2925-2929

  View details for Web of Science ID 000229091300019

  View details for PubMedID 20058329

• Study of J/psi ->omega K+K- PHYSICS LETTERS B Ablikim, M., Bai, J. Z., Ban, Y., Bian, J. G., Bugg, D. V., Cai, X., Chang, J. F., Chen, H. F., Chen, H. S., Chen, H. X., Chen, J. C., Chen, J., Chen, J., CHEN, M. L., Chen, Y. B., Chi, S. P., Chu, Y. P., Cui, X. Z., Dai, H. L., Dai, Y. S., Deng, Z. Y., Dong, L. Y., Dong, Q. F., Du, S. X., Du, Z. Z., Fang, J., Fang, S. S., Fu, C. D., Fu, H. Y., Gao, C. S., Gao, Y. N., Gong, M. Y., Gong, W. X., Gu, S. D., Guo, Y. N., Guo, Y. Q., Guo, Z. J., Harris, F. A., He, K. L., He, M., He, X., Heng, Y. K., Hu, H. M., Hu, T., Huang, G. S., Huang, X. P., Huang, X. T., Ji, X. B., Jiang, C. H., Jiang, X. S., Jin, D. P., Jin, S., Jin, Y., Jin, Y., Lai, Y. F., Li, F., Li, G., Li, H. H., Li, J., Li, J. C., Li, Q. J., Li, R. Y., Li, S. M., Li, W. D., Li, W. G., Li, X. L., Li, X. Q., Li, Y. L., Liang, Y. F., Liao, H. B., Liu, C. X., Liu, F., Liu, F., Liu, H. H., Liu, H. M., Liu, J., Liu, J. B., Liu, J. P., Liu, R. G., Liu, Z. A., Liu, Z. X., Lu, F., Lu, G. R., Lu, H. J., Lu, J. G., Luo, C. L., Luo, L. X., Luo, X. L., Ma, F. C., Ma, H. L., Ma, J. M., Ma, L. L., Ma, Q. M., Ma, X. B., Ma, X. Y., Mao, Z. P., Mo, X. H., Nie, J., Nie, Z. D., Olsen, S. L., Peng, H. P., Qi, N. D., Qian, C. D., Qin, H., Qiu, J. F., Ren, Z. Y., Rong, G., Shan, L. Y., Shang, L., Shen, D. L., Shen, X. Y., Sheng, H. Y., Shi, F., Shi, X., Sun, H. S., Sun, J. F., Sun, S. S., Sun, Y. Z., Sun, Z. J., Tang, X., Tao, N., Tian, Y. R., Tong, G. L., Varner, G. S., Wang, D. Y., Wang, J. Z., Wang, K., Wang, L., Wang, L. S., Wang, M., Wang, P., Wang, P. L., Wang, S. Z., Wang, W. F., Wang, Y. F., Wang, Z., Wang, Z. Y., Wang, Z., Wang, Z., Wei, C. L., Wei, D. H., Wu, N., Wu, Y. M., Xia, X. M., Xie, X. X., Xin, B., Xu, G. F., Xu, H., Xue, S. T., Yan, M. L., Yang, F., Yang, H. X., Yang, J., Yang, Y. X., Ye, M., Ye, M. H., Ye, Y. X., Yi, L. H., Yi, Z. Y., Yu, C. S., Yu, G. W., Yuan, C. Z., Yuan, J. M., Yuan, Y., Zang, S. L., Zeng, Y., Zeng, Y., Zhang, B. X., Zhang, B. Y., Zhang, C. C., Zhang, D. H., Zhang, H. Y., Zhang, J., Zhang, J. W., Zhang, J. Y., Zhang, Q. J., Zhang, S. Q., Zhang, X. M., Zhang, X. Y., Zhang, Y. Y., Zhang, Y. Y., Zhang, Z. P., Zhang, Z. Q., Zhao, D. X., Zhao, J. B., Zhao, J. W., Zhao, M. G., Zhao, P. P., Zhao, W. R., Zhao, X. J., Zhao, Y. B., Zhao, Z. G., Zheng, H. Q., Zheng, J. P., Zheng, L. S., Zheng, Z. P., Zhong, X. C., Zhou, B. Q., Zhou, G. M., Zhou, L., Zhou, N. F., Zhu, K. J., Zhu, Q. M., Zhu, Y. C., Zhu, Y. S., Zhu, Y. C., Zhu, Z. A., Zhuang, B. A., Zhuang, X. A., Zou, B. S. 2004; 603 (3-4): 138-145

  View details for DOI 10.1016/j.physletb.2004.10.030

  View details for Web of Science ID 000225419600006

• Aharonov-bohm interference and beating in single-walled carbon-nanotube interferometers PHYSICAL REVIEW LETTERS Cao, J., Wang, Q., Rolandi, M., Dai, H. J. 2004; 93 (21)

  Abstract

  Relatively low magnetic fields applied parallel to the axis of a chiral single-walled carbon nanotube are found causing large modulations to the p channel or valence band conductance of the nanotube in the Fabry-Perot interference regime. Beating in the Aharonov-Bohm type of interference between two field-induced nondegenerate subbands of spiraling electrons is responsible for the observed modulation with a pseudoperiod much smaller than that needed to reach the flux quantum Phi0 = h/e through the nanotube cross section. We show that single-walled nanotubes represent the smallest cylinders exhibiting the Aharonov-Bohm effect with rich interference and beating phenomena arising from well-defined molecular orbitals reflective of the nanotube chirality.

  View details for DOI 10.1103/PhysRevLett.93.216803

  View details for Web of Science ID 000225220500065

  View details for PubMedID 15601048

• Electric-field-directed growth of carbon nanotubes in two dimensions 48th International Conference on Electron, Ion and Photon Beam Technology and Nanofabrication Nojeh, A., Ural, A., Pease, R. F., DAI, H. J. A V S AMER INST PHYSICS. 2004: 3421–25

  View details for DOI 10.1116/1.1821578

  View details for Web of Science ID 000226439800168

• Electron beam stimulated field-emission from single-walled carbon nanotubes 48th International Conference on Electron, Ion and Photon Beam Technology and Nanofabrication Nojeh, A., Wong, W. K., Yieh, E., Pease, R. F., DAI, H. J. A V S AMER INST PHYSICS. 2004: 3124–27

  View details for DOI 10.1116/1.1809628

  View details for Web of Science ID 000226439800104

• Miniature organic transistors with carbon nanotubes as quasi-one-dimensional electrodes JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Qi, P. F., Javey, A., Rolandi, M., Wang, Q., Yenilmez, E., Dai, H. J. 2004; 126 (38): 11774-11775

  Abstract

  As the dimensions of electronic devices approach those of molecules, the size, geometry, and chemical composition of the contact electrodes play increasingly dominant roles in device functions. It is shown here that single-walled carbon nanotubes (SWNT) can be used as quasi-one-dimensional (1D) electrodes to construct organic field effect transistors (FET) with molecular scale width ( approximately 2 nm) and channel length (1-3 nm). An important feature owing to the quasi-1D electrode geometry is the favorable gate electrostatics that allows for efficient switching of ultra-short organic channels. This affords room temperature conductance modulation by orders of magnitude for organic transistors that are only several molecules in length, with switching characteristics superior to similar devices with lithographically patterned metal electrodes. With nanotubes, covalent carbon-carbon bonds could be utilized to form contacts to molecular materials. The unique geometrical, physical, and chemical properties of carbon nanotube electrodes may lead to various interesting molecular devices.

  View details for DOI 10.1021/ja045900k

  View details for Web of Science ID 000224103900012

  View details for PubMedID 15382895

• Surface chemistry and electrical properties of germanium nanowires JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Wang, D. W., Chang, Y. L., Wang, Q., Cao, J., Farmer, D. B., Gordon, R. G., Dai, H. J. 2004; 126 (37): 11602-11611

  Abstract

  Germanium nanowires (GeNWs) with p- and n-dopants were synthesized by chemical vapor deposition (CVD) and were used to construct complementary field-effect transistors (FETs). Electrical transport and X-ray photoelectron spectroscopy (XPS) data are correlated to glean the effects of Ge surface chemistry to the electrical characteristics of GeNWs. Large hysteresis due to water molecules strongly bound to GeO(2) on GeNWs is revealed. Different oxidation behavior and hysteresis characteristics and opposite band bending due to Fermi level pinning by interface states between Ge and surface oxides are observed for p- and n-type GeNWs. Vacuum annealing above 400 degrees C is used to remove surface oxides and eliminate hysteresis in GeNW FETs. High-kappa dielectric HfO(2) films grown on clean GeNW surfaces by atomic layer deposition (ALD) using an alkylamide precursor is effective in serving as the first layer of surface passivation. Lastly, the depletion length along the radial direction of nanowires is evaluated. The result suggests that surface effects could be dominant over the "bulk" properties of small diameter wires.

  View details for DOI 10.1021/ja047435x

  View details for Web of Science ID 000223921800046

  View details for PubMedID 15366907

• Ten- to 50-nm-long quasi-ballistic carbon nanotube devices obtained without complex lithography PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Javey, A., Qi, P. F., Wang, Q., Dai, H. J. 2004; 101 (37): 13408-13410

  Abstract

  A simple method combining photolithography and shadow (or angle) evaporation is developed to fabricate single-walled carbon nanotube (SWCNT) devices with tube lengths of approximately 10-50 nm between metal contacts. Large numbers of such short devices are obtained without the need of complex tools such as electron beam lithography. Metallic SWCNTs with lengths of approximately 10 nm, near the mean free path of l(op) approximately 15 nm for optical phonon scattering, exhibit nearly ballistic transport at high biases and can carry unprecedented 100-microA currents per tube. Semiconducting SWCNT field-effect transistors with approximately 50-nm channel lengths are routinely produced to achieve quasi-ballistic operations for molecular transistors. The results demonstrate highly length-scaled and high-performance interconnects and transistors realized with SWCNTs.

  View details for DOI 10.1073/pnas.0404450101

  View details for Web of Science ID 000223917900004

  View details for PubMedID 15347810

  View details for PubMedCentralID PMC518770

• Scanning electron microscopy of field-emitting individual single-walled carbon nanotubes APPLIED PHYSICS LETTERS Nojeh, A., Wong, W. K., Baum, A. W., Pease, R. F., Dai, H. 2004; 85 (1): 112-114

  View details for DOI 10.1063/1.1763984

  View details for Web of Science ID 000222360300038

• Self-aligned ballistic molecular transistors and electrically parallel nanotube arrays NANO LETTERS Javey, A., Guo, J., Farmer, D. B., Wang, Q., Yenilmez, E., Gordon, R. G., Lundstrom, M., Dai, H. J. 2004; 4 (7): 1319-1322

  View details for DOI 10.1021/nl049222b

  View details for Web of Science ID 000222762000028

• Nanotube molecular transporters: Internalization of carbon nanotube-protein conjugates into mammalian cells JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Kam, N. W., Jessop, T. C., Wender, P. A., Dai, H. J. 2004; 126 (22): 6850-6851

  Abstract

  The interactions between various functionalized carbon nanotubes and several types of human cancer cells are explored. We have prepared modified nanotubes and have shown that these can be derivatized in a way that enables attachment of small molecules and of proteins, the latter through a novel noncovalent association. The functionalized carbon nanotubes enter nonadherent human cancer cells as well as adherent cell lines (CHO and 3T3) and by themselves are not toxic. While the fluoresceinated protein streptavidin (MW approximately 60 kD) by itself does not enter cells, it readily enters cells when complexed to a nanotube-biotin transporter and exhibits dose-dependent cytotoxicity. The uptake pathway is consistent with adsorption-mediated endocytosis. The use of carbon nanotubes as molecular transporters could be exploited for various cargos. The biocompatibility and unique physical, electrical, optical, and mechanical properties of nanotubes provide the basis for new classes of materials for drug, protein, and gene delivery applications.

  View details for DOI 10.1021/ja0486059

  View details for Web of Science ID 000221828200007

  View details for PubMedID 15174838

• Measurement of ionizing radiation using carbon nanotube field effect transistor 46th Annual Meeting of the American-Association-of-Physicists-in-Medicine Tang, X., Yang, Y., Kim, W., Wang, Q., Xing, L., Dai, H. AMER ASSOC PHYSICISTS MEDICINE AMER INST PHYSICS. 2004: 1839–39

  View details for Web of Science ID 000222259100585

• Dendrimer monolayers as negative and positive tone resists for scanning probe lithography NANO LETTERS Rolandi, M., Suez, I., Dai, H. J., Frechet, J. M. 2004; 4 (5): 889-893

  View details for DOI 10.1021/nl049700i

  View details for Web of Science ID 000221410000026

• Ab initio study of CNT NO2 gas sensor CHEMICAL PHYSICS LETTERS Peng, S., Cho, K. J., Qi, P. F., DAI, H. J. 2004; 387 (4-6): 271-276

  View details for DOI 10.1016/j.cplett.2004.02.026

  View details for Web of Science ID 000220620200013

• Carbon nanotubes: Continued innovations and challenges MRS BULLETIN Dresselhaus, M. S., Dai, H. 2004; 29 (4): 237-239

  View details for Web of Science ID 000220898700018

• Recent advances in methods of forming carbon nanotubes MRS BULLETIN Liu, J., Fan, S. S., Dai, H. J. 2004; 29 (4): 244-250

  View details for Web of Science ID 000220898700019

• Fabrication and characterization of a carbon nanotube microelectrode array for retinal prostheses Annual Meeting of the Association-for-Research-in-Vision-and-Ophthalmology Wang, K., Dai, H., Leng, T., Mehenti, N. Z., Harris, J. S., Fishman, H. A. ASSOC RESEARCH VISION OPHTHALMOLOGY INC. 2004: U379–U379

  View details for Web of Science ID 000223338201366

• Electron transport in short macromolecular carbon nanotubes. 227th National Meeting of the American-Chemical Society Javey, A., DAI, H. J. AMER CHEMICAL SOC. 2004: U260–U260

  View details for Web of Science ID 000223655701347

• Phospholipids-functionalized carbon nanotubes for chemical, biological and electronic applications. 227th National Meeting of the American-Chemical Society Kam, N. W., Kim, W., DAI, H. J. AMER CHEMICAL SOC. 2004: U508–U508

  View details for Web of Science ID 000223655702581

• Semiconducting versus metallic nanotubes: Preferential synthesis or separation. 227th National Meeting of the American-Chemical Society Kim, W., Li, Y. M., DAI, H. J. AMER CHEMICAL SOC. 2004: U1277–U1277

  View details for Web of Science ID 000223655604348

• High-field quasiballistic transport in short carbon nanotubes PHYSICAL REVIEW LETTERS Javey, A., Guo, J., Paulsson, M., Wang, Q., Mann, D., Lundstrom, M., Dai, H. J. 2004; 92 (10)

  Abstract

  Single walled carbon nanotubes with Pd Ohmic contacts and lengths ranging from several microns down to 10 nm are investigated by electron transport experiments and theory. The mean-free path (MFP) for acoustic phonon scattering is estimated to be l(ap) approximately 300 nm, and that for optical phonon scattering is l(op) approximately 15 nm. Transport through very short (approximately 10 nm) nanotubes is free of significant acoustic and optical phonon scattering and thus ballistic and quasiballistic at the low- and high-bias voltage limits, respectively. High currents of up to 70 microA can flow through a short nanotube. Possible mechanisms for the eventual electrical breakdown of short nanotubes at high fields are discussed. The results presented here have important implications to high performance nanotube transistors and interconnects.

  View details for DOI 10.1103/PhysRevLett.92.106804

  View details for Web of Science ID 000220185600040

  View details for PubMedID 15089227

• Carbon nanotube field-effect transistors with integrated ohmic contacts and high-k gate dielectrics NANO LETTERS Javey, A., Guo, J., Farmer, D. B., Wang, Q., Wang, D. W., Gordon, R. G., Lundstrom, M., Dai, H. J. 2004; 4 (3): 447-450

  View details for DOI 10.1021/nl035185x

  View details for Web of Science ID 000220170600013

• An investigation of the mechanisms of electronic sensing of protein adsorption on carbon nanotube devices JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Chen, R. J., Choi, H. C., Bangsaruntip, S., Yenilmez, E., Tang, X. W., Wang, Q., Chang, Y. L., Dai, H. J. 2004; 126 (5): 1563-1568

  Abstract

  It has been reported that protein adsorption on single-walled carbon nanotube field effect transistors (FETs) leads to appreciable changes in the electrical conductance of the devices, a phenomenon that can be exploited for label-free detection of biomolecules with a high potential for miniaturization. This work presents an elucidation of the electronic biosensing mechanisms with a newly developed microarray of nanotube "micromat" sensors. Chemical functionalization schemes are devised to block selected components of the devices from protein adsorption, self-assembled monolayers (SAMs) of methoxy(poly(ethylene glycol))thiol (mPEG-SH) on the metal electrodes (Au, Pd) and PEG-containing surfactants on the nanotubes. Extensive characterization reveals that electronic effects occurring at the metal-nanotube contacts due to protein adsorption constitute a more significant contribution to the electronic biosensing signal than adsorption solely along the exposed lengths of the nanotubes.

  View details for DOI 10.1021/ja038702m

  View details for PubMedID 14759216

• Preferential growth of semiconducting single-walled carbon nanotubes by a plasma enhanced CVD method NANO LETTERS Li, Y. M., Mann, D., Rolandi, M., Kim, W., Ural, A., Hung, S., Javey, A., Cao, J., Wang, D. W., Yenilmez, E., Wang, Q., Gibbons, J. F., Nishi, Y., Dai, H. J. 2004; 4 (2): 317-321

  View details for DOI 10.1021/nl035097c

  View details for Web of Science ID 000188965700025

• Dispatching operation schemes of the three gorges project in cofferdam impoundment period 9th International Symposium on River Sedimentation Dai, H. C., He, W. S. TSINGHUA UNIVERSITY PRESS. 2004: 292–298

  View details for Web of Science ID 000226799100030

• Monolithic integration of carbon nanotube devices with silicon MOS technology NANO LETTERS Tseng, Y. C., Xuan, P. Q., Javey, A., Malloy, R., Wang, Q., Bokor, J., DAI, H. J. 2004; 4 (1): 123-127

  View details for DOI 10.1021/nl0349707

  View details for Web of Science ID 000188233200024

• Germanium nanowire field-effect transistors with SiO2 and high-kappa HfO2 gate dielectrics APPLIED PHYSICS LETTERS Wang, D. W., Wang, Q., Javey, A., Tu, R., Dai, H. J., Kim, H., McIntyre, P. C., Krishnamohan, T., Saraswat, K. C. 2003; 83 (12): 2432-2434

  View details for DOI 10.1063/1.1611644

  View details for Web of Science ID 000185333200044

• Ballistic carbon nanotube field-effect transistors NATURE Javey, A., Guo, J., Wang, Q., Lundstrom, M., Dai, H. J. 2003; 424 (6949): 654-657

  Abstract

  A common feature of the single-walled carbon-nanotube field-effect transistors fabricated to date has been the presence of a Schottky barrier at the nanotube--metal junctions. These energy barriers severely limit transistor conductance in the 'ON' state, and reduce the current delivery capability--a key determinant of device performance. Here we show that contacting semiconducting single-walled nanotubes by palladium, a noble metal with high work function and good wetting interactions with nanotubes, greatly reduces or eliminates the barriers for transport through the valence band of nanotubes. In situ modification of the electrode work function by hydrogen is carried out to shed light on the nature of the contacts. With Pd contacts, the 'ON' states of semiconducting nanotubes can behave like ohmically contacted ballistic metallic tubes, exhibiting room-temperature conductance near the ballistic transport limit of 4e(2)/h (refs 4-6), high current-carrying capability (approximately 25 micro A per tube), and Fabry-Perot interferences at low temperatures. Under high voltage operation, the current saturation appears to be set by backscattering of the charge carriers by optical phonons. High-performance ballistic nanotube field-effect transistors with zero or slightly negative Schottky barriers are thus realized.

  View details for DOI 10.1038/nature01797

  View details for PubMedID 12904787

• Noncovalent functionalization of carbon nanotubes for highly specific electronic biosensors PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA Chen, R. J., Bangsaruntip, S., Drouvalakis, K. A., Kam, N. W., Shim, M., Li, Y. M., Kim, W., Utz, P. J., DAI, H. J. 2003; 100 (9): 4984-4989

  Abstract

  Novel nanomaterials for bioassay applications represent a rapidly progressing field of nanotechnology and nanobiotechnology. Here, we present an exploration of single-walled carbon nanotubes as a platform for investigating surface-protein and protein-protein binding and developing highly specific electronic biomolecule detectors. Nonspecific binding on nanotubes, a phenomenon found with a wide range of proteins, is overcome by immobilization of polyethylene oxide chains. A general approach is then advanced to enable the selective recognition and binding of target proteins by conjugation of their specific receptors to polyethylene oxide-functionalized nanotubes. This scheme, combined with the sensitivity of nanotube electronic devices, enables highly specific electronic sensors for detecting clinically important biomolecules such as antibodies associated with human autoimmune diseases.

  View details for DOI 10.1073/pnas.0837064100

  View details for PubMedID 12697899

• Electromechanical properties of metallic, quasimetallic, and semiconducting carbon nanotubes under stretching PHYSICAL REVIEW LETTERS Cao, J., Wang, Q., Dai, H. J. 2003; 90 (15)

  Abstract

  An electromechanical system is constructed to explore the electrical properties of various types of suspended single-walled carbon nanotubes under the influence of tensile stretching. Small band-gap semiconducting (or quasimetallic) nanotubes exhibit the largest resistance changes and piezoresistive gauge factors ( approximately 600 to 1000) under axial strains. Metallic nanotubes exhibit much weaker but nonzero sensitivity. Comparison between experiments and theoretical predictions and potential applications of nanotube electromechanical systems for physical sensors (e.g., strain gauges, pressure sensors, etc.) are discussed.

  View details for DOI 10.1103/PhysRevLett.90.157601

  View details for Web of Science ID 000182320200049

  View details for PubMedID 12732069

• Controlled polymerization methods for the synthesis of novel polymer architectures and materials. 225th National Meeting of the American-Chemical-Society Waymouth, R. M., Bowden, N. B., Willets, K. A., Gomez, F. J., Chen, R., Gavranovic, G., Fuller, G. G., DAI, H. J., HEDRICK, J. L., Hawker, C. J. AMER CHEMICAL SOC. 2003: U589–U589

  View details for Web of Science ID 000187918003090

• Toward Large Arrays of Multiplex Functionalized Carbon Nanotube Sensors for Highly Sensitive and Selective Molecular Detection. Nano letters Qi, P., Vermesh, O., Grecu, M., Javey, A., Wang, Q., Dai, H., Peng, S., Cho, K. J. 2003; 3 (3): 347-351

  Abstract

  Arrays of electrical devices with each comprising multiple single-walled carbon nanotubes (SWNT) bridging metal electrodes are obtained by chemical vapor deposition (CVD) of nanotubes across prefabricated electrode arrays. The ensemble of nanotubes in such a device collectively exhibits large electrical conductance changes under electrostatic gating, owing to the high percentage of semiconducting nanotubes. This leads to the fabrication of large arrays of low-noise electrical nanotube sensors with 100% yield for detecting gas molecules. Polymer functionalization is used to impart high sensitivity and selectivity to the sensors. Polyethyleneimine coating affords n-type nanotube devices capable of detecting NO2 at less than 1 ppb (parts-per-billion) concentrations while being insensitive to NH3. Coating Nafion (a polymeric perfluorinated sulfonic acid ionomer) on nanotubes blocks NO2 and allows for selective sensing of NH3. Multiplex functionalization of a nanotube sensor array is carried out by microspotting. Detection of molecules in a gas mixture is demonstrated with the multiplexed nanotube sensors.

  View details for DOI 10.1021/nl034010k

  View details for PubMedID 36517998

• Spontaneous and selective formation of quantum dots on single-walled carbon nanotube surfaces 225th National Meeting of the American-Chemical-Society Choi, H. C., DAI, H. J. AMER CHEMICAL SOC. 2003: U16–U16

  View details for Web of Science ID 000187918000061

• Toward large arrays of multiplex functionalized carbon nanotube sensors for highly sensitive and selective molecular detection NANO LETTERS Pengfei, Q. F., Vermesh, O., Grecu, M., Javey, A., Wang, O., Dai, H. J., Peng, S., Cho, K. J. 2003; 3 (3): 347-351

  View details for DOI 10.1021/nl034010k

  View details for Web of Science ID 000181586600015

• Ring opening metathesis polymerization on non-covalently functionalized single-walled carbon nanotubes CHEMICAL COMMUNICATIONS Gomez, F. J., Chen, R. J., Wang, D. W., Waymouth, R. M., Dai, H. J. 2003: 190-191

  Abstract

  Norbornene polymerization has been initiated selectively on the surface of single-walled carbon nanotubes (SWNTs) via a specifically adsorbed pyrene-linked ROMP initiator, resulting in a homogeneous non-covalent poly(norbornene) coating.

  View details for DOI 10.1039/b211194b

  View details for PubMedID 12585385

• Advancements in complementary carbon nanotube field-effect transistors IEEE International Electron Devices Meeting Javey, A., Wang, Q., Kim, W., Dai, H. J. IEEE. 2003: 741–744

  View details for Web of Science ID 000189158800169

• Delivery of catalytic metal species onto surfaces with dendrimer carriers for the synthesis of carbon nanotubes with narrow diameter distribution JOURNAL OF PHYSICAL CHEMISTRY B Choi, H. C., Kim, W., Wang, D. W., Dai, H. J. 2002; 106 (48): 12361-12365

  View details for DOI 10.1021/jp026421f

  View details for Web of Science ID 000179618200001

• High-kappa dielectrics for advanced carbon-nanotube transistors and logic gates NATURE MATERIALS Javey, A., Kim, H., Brink, M., Wang, Q., Ural, A., Guo, J., McIntyre, P., McEuen, P., Lundstrom, M., DAI, H. J. 2002; 1 (4): 241-246

  Abstract

  The integration of materials having a high dielectric constant (high-kappa) into carbon-nanotube transistors promises to push the performance limit for molecular electronics. Here, high-kappa (approximately 25) zirconium oxide thin-films (approximately 8 nm) are formed on top of individual single-walled carbon nanotubes by atomic-layer deposition and used as gate dielectrics for nanotube field-effect transistors. The p-type transistors exhibit subthreshold swings of S approximately 70 mV per decade, approaching the room-temperature theoretical limit for field-effect transistors. Key transistor performance parameters, transconductance and carrier mobility reach 6,000 S x m(-1) (12 microS per tube) and 3,000 cm2 x V(-1) x s(-1) respectively. N-type field-effect transistors obtained by annealing the devices in hydrogen exhibit S approximately 90 mV per decade. High voltage gains of up to 60 are obtained for complementary nanotube-based inverters. The atomic-layer deposition process affords gate insulators with high capacitance while being chemically benign to nanotubes, a key to the integration of advanced dielectrics into molecular electronics.

  View details for DOI 10.1038/nmat769

  View details for PubMedID 12618786

• Carbon nanotubes: Synthesis, integration, and properties ACCOUNTS OF CHEMICAL RESEARCH DAI, H. J. 2002; 35 (12): 1035-1044

  Abstract

  Synthesis of carbon nanotubes by chemical vapor deposition over patterned catalyst arrays leads to nanotubes grown from specific sites on surfaces. The growth directions of the nanotubes can be controlled by van der Waals self-assembly forces and applied electric fields. The patterned growth approach is feasible with discrete catalytic nanoparticles and scalable on large wafers for massive arrays of novel nanowires. Controlled synthesis of nanotubes opens up exciting opportunities in nanoscience and nanotechnology, including electrical, mechanical, and electromechanical properties and devices, chemical functionalization, surface chemistry and photochemistry, molecular sensors, and interfacing with soft biological systems.

  View details for DOI 10.1021/ar0101640

  View details for Web of Science ID 000179918200006

  View details for PubMedID 12484791

• Electric-field-aligned growth of single-walled carbon nanotubes on surfaces APPLIED PHYSICS LETTERS Ural, A., Li, Y. M., Dai, H. J. 2002; 81 (18): 3464-3466

  View details for DOI 10.1063/1.1518773

  View details for Web of Science ID 000178881800052

• Carbon nanotube transistor arrays for multistage complementary logic and ring oscillators NANO LETTERS Javey, A., Wang, Q., Ural, A., Li, Y. M., Dai, H. J. 2002; 2 (9): 929-932

  View details for DOI 10.1021/nl025647r

  View details for Web of Science ID 000178010900004

• Ordered nanomaterial architectures: Carbon nanotubes. Dai, H. AMER CHEMICAL SOC. 2002: U318–U318

  View details for Web of Science ID 000177422201578

• Nanoparticles and carbon nanotubes synthesis. Dai, H. J. AMER CHEMICAL SOC. 2002: U308–U308

  View details for Web of Science ID 000177422301591

• Spontaneous reduction of metal ions on the sidewalls of carbon nanotubes JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Choi, H. C., Shim, M., Bangsaruntip, S., Dai, H. J. 2002; 124 (31): 9058-9059

  Abstract

  Nanotube/nanoparticle hybrid structures are prepared by forming Au and Pt nanoparticles on the sidewalls of single-walled carbon nanotubes. Reducing agent or catalyst-free electroless deposition, which purely utilizes the redox potential difference between Au3+, Pt2+, and the carbon nanotube, is the main driving force for this reaction. It is also shown that carbon nanotubes act as a template for wire-like metal structures. The successful formation of the hybrid structures is monitored by atomic force microscopy (AFM) and electrical measurements.

  View details for DOI 10.1021/ja026824t

  View details for Web of Science ID 000177209500027

  View details for PubMedID 12149003

• Integration of suspended carbon nanotube arrays into electronic devices and electromechanical systems APPLIED PHYSICS LETTERS Franklin, N. R., Wang, Q., Tombler, T. W., Javey, A., Shim, M., Dai, H. J. 2002; 81 (5): 913-915

  View details for DOI 10.1063/1.1497710

  View details for Web of Science ID 000177008900043

• Synthesis of ultralong and high percentage of semiconducting single-walled carbon nanotubes NANO LETTERS Kim, W., Choi, H. C., Shim, M., Li, Y. M., Wang, D. W., Dai, H. J. 2002; 2 (7): 703-708

  View details for DOI 10.1021/nl025602q

  View details for Web of Science ID 000176827500006

• Carbon nanotube as a model system for nanoscale science. Dai, H. J. AMER CHEMICAL SOC. 2002: C46–C46

  View details for Web of Science ID 000176296801628

• Functionalization of carbon nanotubes for biocompatibility and biomolecular recognition NANO LETTERS Shim, M., Kam, N. W., Chen, R. J., Li, Y. M., Dai, H. J. 2002; 2 (4): 285-288

  View details for DOI 10.1021/nl015692j

  View details for Web of Science ID 000175041800006

• Wafer scale production of carbon nanotube scanning probe tips for atomic force microscopy APPLIED PHYSICS LETTERS Yenilmez, E., Wang, Q., Chen, R. J., Wang, D. W., Dai, H. J. 2002; 80 (12): 2225-2227

  View details for DOI 10.1063/1.1464227

  View details for Web of Science ID 000174498700061

• Carbon nanotubes: opportunities and challenges SURFACE SCIENCE Dai, H. J. 2002; 500 (1-3): 218-241

  View details for Web of Science ID 000175303400011

• Imaging as-grown single-walled carbon nanotubes originated from isolated catalytic nanoparticles APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING Zhang, Y., Li, Y., Kim, W., Wang, D., Dai, H. 2002; 74 (3): 325-328

  View details for DOI 10.1007/s003390201274

  View details for Web of Science ID 000174611600001

• Electrical properties and devices of large-diameter single-walled carbon nanotubes APPLIED PHYSICS LETTERS Javey, A., Shim, M., Dai, H. J. 2002; 80 (6): 1064-1066

  View details for Web of Science ID 000173612900054

• A new scanning probe lithography scheme with a novel metal resist ADVANCED MATERIALS Rolandi, M., Quate, C. F., Dai, H. J. 2002; 14 (3): 191-?

  View details for Web of Science ID 000173839000002

• Chemical profiling of single nanotubes: Intramolecular p-n-p junctions and on-tube single-electron transistors APPLIED PHYSICS LETTERS Kong, J., Cao, J., Dai, H. J., Anderson, E. 2002; 80 (1): 73-75

  View details for Web of Science ID 000173029000025

• Low-temperature synthesis of single-crystal germanium nanowires by chemical vapor deposition ANGEWANDTE CHEMIE-INTERNATIONAL EDITION Wang, D. W., DAI, H. J. 2002; 41 (24): 4783-4786

  View details for Web of Science ID 000180051600048

  View details for PubMedID 12481357

• Patterned growth of single-walled carbon nanotubes on full 4-inch wafers APPLIED PHYSICS LETTERS Franklin, N. R., Li, Y. M., Chen, R. J., Javey, A., Dai, H. J. 2001; 79 (27): 4571-4573

  View details for Web of Science ID 000172835400032

• Polymer functionalization for air-stable n-type carbon nanotube field-effect transistors JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Shim, M., Javey, A., Kam, N. W., DAI, H. J. 2001; 123 (46): 11512-11513

  View details for DOI 10.1021/ja0169670

  View details for Web of Science ID 000172240100037

  View details for PubMedID 11707143

• Molecular photodesorption from single-walled carbon nanotubes APPLIED PHYSICS LETTERS Chen, R. J., Franklin, N. R., Kong, J., Cao, J., Tombler, T. W., Zhang, Y. G., Dai, H. J. 2001; 79 (14): 2258-2260

  View details for Web of Science ID 000171134900045

• Functionalized carbon nanotubes for molecular hydrogen sensors ADVANCED MATERIALS Kong, J., Chapline, M. G., DAI, H. J. 2001; 13 (18): 1384-1386

  View details for Web of Science ID 000171156800008

• Quantum interference and ballistic transmission in nanotube electron waveguides PHYSICAL REVIEW LETTERS Kong, J., Yenilmez, E., Tombler, T. W., Kim, W., DAI, H. J., Laughlin, R. B., Liu, L., Jayanthi, C. S., Wu, S. Y. 2001; 87 (10)

  Abstract

  The electron transport properties of well-contacted individual single-walled carbon nanotubes are investigated in the ballistic regime. Phase coherent transport and electron interference manifest as conductance fluctuations as a function of Fermi energy. Resonance with standing waves in finite-length tubes and localized states due to imperfections are observed for various Fermi energies. Two units of quantum conductance 2G(0) = 4e(2)/h are measured for the first time, corresponding to the maximum conductance limit for ballistic transport in two channels of a nanotube.

  View details for DOI 10.1103/PhysRevLett.87.106801

  View details for Web of Science ID 000170901300030

  View details for PubMedID 11531494

• Noncovalent sidewall functionalization of single-walled carbon nanotubes for protein immobilization JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Chen, R. J., Zhang, Y. G., Wang, D. W., DAI, H. J. 2001; 123 (16): 3838-3839

  View details for DOI 10.1021/ja010172b

  View details for Web of Science ID 000168442500032

  View details for PubMedID 11457124

• Integrated nanotubes for chemical sensors. Dai, H. J. AMER CHEMICAL SOC. 2001: U380–U381

  View details for Web of Science ID 000168824702719

• Nanotube growth and characterization CARBON NANOTUBES Dai, H. J. 2001; 80: 29-53

  View details for Web of Science ID 000170063800003

• Modulated chemical doping of individual carbon nanotubes SCIENCE Zhou, C. W., Kong, J., Yenilmez, E., DAI, H. J. 2000; 290 (5496): 1552-1555

  Abstract

  Modulation doping of a semiconducting single-walled carbon nanotube along its length leads to an intramolecular wire electronic device. The nanotube is doped n-type for half of its length and p-type for the other half. Electrostatic gating can tune the system into p-n junctions, causing it to exhibit rectifying characteristics or negative differential conductance. The system can also be tuned into n-type, exhibiting single-electron charging and negative differential conductance at low temperatures. The low-temperature behavior is manifested by a quantum dot formed by chemical inhomogeneity along the tube.

  View details for Web of Science ID 000165446200043

  View details for PubMedID 11090348

• Metal coating on suspended carbon nanotubes and its implication to metal-tube interaction CHEMICAL PHYSICS LETTERS Zhang, Y., Franklin, N. W., Chen, R. J., Dai, H. J. 2000; 331 (1): 35-41

  View details for Web of Science ID 000165515100007

• An enhanced CVD approach to extensive nanotube networks with directionality ADVANCED MATERIALS Franklin, N. R., DAI, H. J. 2000; 12 (12): 890-894

  View details for Web of Science ID 000087851400007

• Reversible electromechanical characteristics of carbon nanotubes under local-probe manipulation Nature Tombler, T. W., Zhou, C., Alexseyev, L., Kong, J., Dai, H., Liu, L., Jayanthi, C. S., Tang, M., Wu, S. Y. 2000; 405 (6788): 769-72

  Abstract

  The effects of mechanical deformation on the electrical properties of carbon nanotubes are of interest given the practical potential of nanotubes in electromechanical devices, and they have been studied using both theoretical and experimental approaches. One recent experiment used the tip of an atomic force microscope (AFM) to manipulate multi-walled nanotubes, revealing that changes in the sample resistance were small unless the nanotubes fractured or the metal-tube contacts were perturbed. But it remains unclear how mechanical deformation affects the intrinsic electrical properties of nanotubes. Here we report an experimental and theoretical elucidation of the electromechanical characteristics of individual single-walled carbon nanotubes (SWNTs) under local-probe manipulation. We use AFM tips to deflect suspended SWNTs reversibly, without changing the contact resistance; in situ electrical measurements reveal that the conductance of an SWNT sample can be reduced by two orders of magnitude when deformed by an AFM tip. Our tight-binding simulations indicate that this effect is owing to the formation of local sp3 bonds caused by the mechanical pushing action of the tip.

  View details for DOI 10.1038/35015519

  View details for PubMedID 10866192

• Intrinsic electrical properties of individual single-walled carbon nanotubes with small band gaps Physical review letters Zhou, C., Kong, J., Dai, H. 2000; 84 (24): 5604-7

  Abstract

  Individual single-walled carbon nanotubes (SWNT) exhibiting small band gaps on the order of 10 meV are observed for the first time in electron transport measurements. Transport through the valence or conduction band of a small-gap semiconducting SWNT (SGS-SWNT) can be tuned by a nearby gate voltage. Intrinsic electrical properties of the Ohmically contacted SGS-SWNT are elucidated. An SGS-SWNT exhibits metal- or semiconductorlike characteristics depending on the Fermi level position in the band structure.

  View details for PubMedID 10991005

• Controlling nanotube growth PHYSICS WORLD DAI, H. J. 2000; 13 (6): 43-47

  View details for Web of Science ID 000087479000029

• Superconducting proximity effect in single-wall carbon nanotubes 22nd International Conference on Low Temperature Physics Morpurgo, A. F., Kong, J., Marcus, C. M., Dai, H. ELSEVIER SCIENCE BV. 2000: 382–83

  View details for Web of Science ID 000086333700107

• Electrical measurements of individual semiconducting single-walled carbon nanotubes of various diameters APPLIED PHYSICS LETTERS Zhou, C. W., Kong, J., Dai, H. J. 2000; 76 (12): 1597-1599

  View details for Web of Science ID 000085857100037

• Nanotube molecular wires as chemical sensors Science (New York, N.Y.) Kong, J., Franklin, N. R., Zhou, C., Chapline, M. G., Peng, S., Cho, K., Dai, H. 2000; 287 (5453): 622-5

  Abstract

  Chemical sensors based on individual single-walled carbon nanotubes (SWNTs) are demonstrated. Upon exposure to gaseous molecules such as NO(2) or NH(3), the electrical resistance of a semiconducting SWNT is found to dramatically increase or decrease. This serves as the basis for nanotube molecular sensors. The nanotube sensors exhibit a fast response and a substantially higher sensitivity than that of existing solid-state sensors at room temperature. Sensor reversibility is achieved by slow recovery under ambient conditions or by heating to high temperatures. The interactions between molecular species and SWNTs and the mechanisms of molecular sensing with nanotube molecular wires are investigated.

  View details for PubMedID 10649989

• Nanotube molecular wires as chemical sensors SCIENCE Kong, J., Franklin, N. R., Zhou, C. W., Chapline, M. G., Peng, S., Cho, K. J., DAI, H. J. 2000; 287 (5453): 622-625

  Abstract

  Chemical sensors based on individual single-walled carbon nanotubes (SWNTs) are demonstrated. Upon exposure to gaseous molecules such as NO(2) or NH(3), the electrical resistance of a semiconducting SWNT is found to dramatically increase or decrease. This serves as the basis for nanotube molecular sensors. The nanotube sensors exhibit a fast response and a substantially higher sensitivity than that of existing solid-state sensors at room temperature. Sensor reversibility is achieved by slow recovery under ambient conditions or by heating to high temperatures. The interactions between molecular species and SWNTs and the mechanisms of molecular sensing with nanotube molecular wires are investigated.

  View details for Web of Science ID 000084989400038

• Terabit-per-square-inch data storage with the atomic force microscope APPLIED PHYSICS LETTERS Cooper, E. B., Manalis, S. R., Fang, H., Dai, H., Matsumoto, K., Minne, S. C., Hunt, T., Quate, C. F. 1999; 75 (22): 3566-3568

  View details for Web of Science ID 000083845800044

• Gate-Controlled Superconducting Proximity Effect in Carbon Nanotubes. Science (New York, N.Y.) Morpurgo, A. F., Kong, J., Marcus, C. M., Dai, H. 1999; 286 (5438): 263-265

  Abstract

  The superconducting proximity effect in single-walled carbon nanotubes connected to niobium electrodes was controlled with the use of nearby gates that tune the niobium-nanotube transparency. At 4.2 kelvin, when the transparency was tuned to be high, a dip in the low-bias differential resistance was observed, indicating a proximity effect mediated by Andreev reflection. When the transparency was tuned to be low, signatures of Andreev reflection disappeared and only tunneling conduction was observed. Below approximately 4 kelvin, a narrow peak in differential resistance around zero bias appeared superimposed on the Andreev dip, probably as a result of electron-electron interaction competing with the proximity effect.

  View details for PubMedID 10514364

• Gate-controlled superconducting proximity effect in carbon nanotubes SCIENCE Morpurgo, A. F., Kong, J., Marcus, C. M., Dai, H. 1999; 286 (5438): 263-265

  View details for Web of Science ID 000083024400036

• Directed growth of free-standingsingle-walled carbon nanotubes JOURNAL OF THE AMERICAN CHEMICAL SOCIETY Cassell, A. M., Franklin, N. R., Tombler, T. W., Chan, E. M., Han, J., DAI, H. J. 1999; 121 (34): 7975-7976

  View details for Web of Science ID 000082471100045

• Synthesis, integration, and electrical properties of individual single-walled carbon nanotubes APPLIED PHYSICS A-MATERIALS SCIENCE & PROCESSING Kong, J., Zhou, C., Morpurgo, A., Soh, H. T., Quate, C. F., Marcus, C., Dai, H. 1999; 69 (3): 305-308

  View details for Web of Science ID 000082304200008

• Integrated nanotube circuits: Controlled growth and ohmic contacting of single-walled carbon nanotubes APPLIED PHYSICS LETTERS Soh, H. T., Quate, C. F., Morpurgo, A. F., Marcus, C. M., Kong, J., Dai, H. J. 1999; 75 (5): 627-629

  View details for Web of Science ID 000081644100011

• Carbon nanotubes as AFM tips: Measuring DNA molecules at the liquid/solid interface Asia-Pacific Surface and Interface Analysis Conference 1998 (APSIAC 98) Li, J., Cassell, A. M., DAI, H. J. WILEY-BLACKWELL. 1999: 8–11

  View details for Web of Science ID 000082482200003

• Self-oriented regular arrays of carbon nanotubes and their field emission properties Science (New York, N.Y.) Fan, S., Chapline, M. G., Franklin, N. R., Tombler, T. W., Cassell, A. M., Dai, H. 1999; 283 (5401): 512-4

  Abstract

  The synthesis of massive arrays of monodispersed carbon nanotubes that are self-oriented on patterned porous silicon and plain silicon substrates is reported. The approach involves chemical vapor deposition, catalytic particle size control by substrate design, nanotube positioning by patterning, and nanotube self-assembly for orientation. The mechanisms of nanotube growth and self-orientation are elucidated. The well-ordered nanotubes can be used as electron field emission arrays. Scaling up of the synthesis process should be entirely compatible with the existing semiconductor processes, and should allow the development of nanotube devices integrated into silicon technology.

  View details for PubMedID 9915692

• Self-oriented regular arrays of carbon nanotubes and their field emission properties SCIENCE Fan, S. S., Chapline, M. G., Franklin, N. R., Tombler, T. W., Cassell, A. M., DAI, H. J. 1999; 283 (5401): 512-514

  View details for Web of Science ID 000078203300028

• Synthesis of individual single-walled carbon nanotubes on patterned silicon wafers NATURE Kong, J., Soh, H. T., Cassell, A. M., Quate, C. F., Dai, H. J. 1998; 395 (6705): 878-881

  View details for Web of Science ID 000076713400050

• Exploiting the properties of carbon nanotubes for nanolithography APPLIED PHYSICS LETTERS Dai, H. J., Franklin, N., Han, J. 1998; 73 (11): 1508-1510

  View details for Web of Science ID 000075861100018

• Chemical vapor deposition of methane for single-walled carbon nanotubes CHEMICAL PHYSICS LETTERS Kong, J., Cassell, A. M., Dai, H. J. 1998; 292 (4-6): 567-574

  View details for Web of Science ID 000075482300030

• Cellulose acetate hollow fiber performance for ultra-low pressure reverse osmosis International Congress on Membranes and Membrane Processes Hao, J. H., Dai, H. P., Yang, P. C., Wei, J. M., Wang, Z. ELSEVIER SCIENCE BV. 1996: 217–21

  View details for Web of Science ID A1996WC55600003

• Atmospheric studies using the High-Resolution Fly's Eye xenon flasher array Conference on Ultraviolet Atmospheric and Space Remote Sensing - Methods and Instrumentation Wiencke, L. R., Bird, D. J., Chen, G. F., Clay, R. W., Dai, H. Y., Dawson, B. R., Huang, M. A., Jui, C. C., Kidd, M. J., Kieda, D. B., Ko, S., Larsen, C. G., Loh, E. C., Smith, J. D., Sokolsky, P., Sommers, P., Tang, J. K., Thomas, S. B., Wilkinson, C. R., Yoshida, S. SPIE - INT SOC OPTICAL ENGINEERING. 1996: 241–251

  View details for Web of Science ID A1996BG73K00021

• An analysis of criteria for the evaluation of learning performance 1996 Australian/New-Zealand Conference on Intelligent Information Systems (ANZIIS 96) Dai, H. H., Liu, J., Ciesielski, V. I E E E. 1996: 84–87

  View details for Web of Science ID A1996BH40F00021

• Actively controlled forced-steering bogie and its H-infinity controller 5th Mini Conference on Vehicle System Dynamics, Identification and Anomalies (VSDIA 96) Dai, H. Y., SHEN, Z. Y. BUDAPEST UNIV TECHNOLOGY ECONOMICS. 1996: 133–140

  View details for Web of Science ID 000080751100011

• Component observations of 10(17) eV EAS with the CASA-MIA and HiRes detectors 24th International Cosmic Ray Conference (XXIV ICRC) Bird, D. J., Borione, A., Boyer, J., Catanese, M., Chen, G. F., Clay, R. W., Covault, C. E., Cronin, J. W., Dai, H. Y., Dawson, B. R., Elbert, J. W., Fick, B. E., Fortson, L. F., Gibbs, K. G., Green, K. D., Glasmacher, M. A., Ho, Y., Huang, A., Jui, C. C., Kidd, M. J., Kieda, D. B., Knapp, B. C., Ko, S., Larsen, C. G., Lee, W., Loh, E. C., Mannel, E. J., Matthews, J., Newport, B. J., Nitz, D., OHALLORAN, T. A., Ong, R. A., Sinclair, D., Smith, J. D., Sokolsky, P., Sommers, P., Tang, J. K., Thomas, S. B., VANDERVELDE, J. C., Wiencke, L. R., Wilkinson, C. R., Yoshida, S. ARGALIA EDITORE DELLE ARTI GRAFICHE EDITORIALI SRL. 1995: 760–763

  View details for Web of Science ID A1995BG94C00200

• Atmospheric monitoring for fluorescence detector experiments 24th International Cosmic Ray Conference (XXIV ICRC) Bird, D. J., Boyer, J., Chen, G. F., Dai, H. Y., Dawson, B. R., Elbert, J. W., Ho, Y., Huang, M. A., Jui, C. C., Kidd, M. J., Kieda, D. B., Ko, S., Larsen, C. G., Loh, E. C., Mannel, E. J., Smith, J. D., Sokolsky, P., Sommers, P., Tang, J. K., Thomas, S. B., Wiencke, L. R., Wilkinson, C. R., Yoshida, S. ARGALIA EDITORE DELLE ARTI GRAFICHE EDITORIALI SRL. 1995: 560–563

  View details for Web of Science ID A1995BG94D00142

• The High Resolution Fly's Eye Project 24th International Cosmic Ray Conference (XXIV ICRC) Bird, D. J., Boyer, J., Chen, G. F., Clay, R. W., Dai, H. Y., Dawson, B. R., Elbert, J. W., Ho, Y., Huang, A., Jui, C. C., Kidd, M. J., Kieda, D. B., Knapp, B. C., Ko, S., Larsen, C. G., Lee, W., Loh, E. C., MANNEL, E., OHALLORAN, T. A., Smith, J. D., Sokolsky, P., Sommers, P., Tang, J. K., Thomas, S. B., Wiencke, L. R., Wilkinson, C. R., Yoshida, S. ARGALIA EDITORE DELLE ARTI GRAFICHE EDITORIALI SRL. 1995: 504–507

  View details for Web of Science ID A1995BG94D00128

• The HiRes2 prototype and coincident measurement with HiRes1 24th International Cosmic Ray Conference (XXIV ICRC) Bird, D. J., Boyer, J., Chen, G. F., Clay, R. W., Dai, H. Y., Dawson, B. R., Ho, Y., Huang, A., Jui, C. C., Kidd, M. J., Kieda, D. B., Knapp, B. C., Ko, S., Larsen, C. G., Loh, E. C., Mannel, E. J., Smith, J. D., Sokolsky, P., Sommers, P., Tang, J. K., Thomas, S. B., Wiencke, L. R., Wilkinson, C. R., Yoshida, S. ARGALIA EDITORE DELLE ARTI GRAFICHE EDITORIALI SRL. 1995: 548–551

  View details for Web of Science ID A1995BG94D00139

• The use of GPS clocks for high relative timing accuracy between HiRes sites 24th International Cosmic Ray Conference (XXIV ICRC) Bird, D. J., Boyer, J., Chen, G. F., Clay, R. W., Dai, H. Y., Dawson, B. R., Elbert, J. W., Ho, Y., Huang, M. A., Jui, C. C., Kidd, M. J., Kieda, D. B., Ko, S., Larsen, C. G., Loh, E. C., Mannel, E. J., OHALLORAN, T. A., Smith, J. D., Sokolsky, P., Sommers, P., Tang, J. K., Thomas, S. B., Wiencke, L. R., Wilkinson, C. R., Yoshida, S. ARGALIA EDITORE DELLE ARTI GRAFICHE EDITORIALI SRL. 1995: 746–749

  View details for Web of Science ID A1995BG94D00189

• Preliminary analysis of monocular HiRes prototype data 24th International Cosmic Ray Conference (XXIV ICRC) Bird, D. J., Boyer, J., Chen, G. F., Dai, H. Y., Dawson, B. R., Elbert, J. W., Ho, Y., Huang, M. A., Jui, C. C., Kidd, M. J., Kieda, D. B., Ko, S., Larsen, C. G., Loh, E. C., Mannel, E. J., OHALLORAN, T. A., Smith, J. D., Sokolsky, P., Sommers, P., Tang, J. K., Thomas, S. B., Wiencke, L. R., Wilkinson, C. R., Yoshida, S. ARGALIA EDITORE DELLE ARTI GRAFICHE EDITORIALI SRL. 1995: 500–503

  View details for Web of Science ID A1995BG94D00127

• Re-examination on primary cosmic ray composition above 10(17) eV 24th International Cosmic Ray Conference (XXIV ICRC) Dai, H. Y., Ding, L. K., Jing, C. L., Jing, G. R., Loh, E. C., Ren, J. L., Zhu, Q. Q. ARGALIA EDITORE DELLE ARTI GRAFICHE EDITORIALI SRL. 1995: 672–675

  View details for Web of Science ID A1995BG94C00175