Lukas Michalek

All Publications

• Electrochemical formation of bis(fluorosulfonyl)imide-derived solid-electrolyte interphase at Li-metal potential. Nature chemistry Yu, W., Lin, K. Y., Boyle, D. T., Tang, M. T., Cui, Y., Chen, Y., Yu, Z., Xu, R., Lin, Y., Feng, G., Huang, Z., Michalek, L., Li, W., Harris, S. J., Jiang, J. C., Abild-Pedersen, F., Qin, J., Cui, Y., Bao, Z. 2024

  Abstract

  Lithium bis(fluorosulfonyl)imide-based liquid electrolytes are promising for realizing high coulombic efficiency and long cycle life in next-generation Li-metal batteries. However, the role of anions in the formation of the solid-electrolyte interphase remains unclear. Here we combine electrochemical analyses and X-ray photoelectron spectroscopy measurements, both with and without sample washing, together with computational simulations, to propose the reaction pathways of electrolyte decomposition and correlate the interphase component solubility with the efficacy of passivation. We discover that not all the products derived from interphase-forming reactions are incorporated into the resulting passivation layer, with a notable portion present in the liquid electrolyte. We also find that the high-performance electrolytes can afford a sufficiently passivating interphase with minimized electrolyte decomposition, by incorporating more anion-decomposition products. Overall, this work presents a systematic approach of coupling electrochemical and surface analyses to paint a comprehensive picture of solid-electrolyte interphase formation, while identifying the key attributes of high-performance electrolytes to guide future designs.

  View details for DOI 10.1038/s41557-024-01689-5

  View details for PubMedID 39622915

  View details for PubMedCentralID 6538711

• A Transparent, Patternable, and Stretchable Conducting Polymer Solid Electrode for Dielectric Elastomer Actuators ADVANCED FUNCTIONAL MATERIALS Kim, E., Lai, J., Michalek, L., Wang, W., Xu, C., Lyu, H., Yu, W., Park, H., Tomo, Y., Root, S. E., Lee, B., Park, J., Park, B., Wei, S., Zhao, C., Bao, Z. 2024

  View details for DOI 10.1002/adfm.202411880

  View details for Web of Science ID 001300258000001

• Printable, stretchable metal-vapor-desorption layers for high-fidelity patterning in soft, freeform electronics. Nature communications Jeong, S., Yoon, H., Michalek, L. F., Kim, G., Kim, J., Seo, J., Kim, D., Park, H., Lee, B., Hong, Y. 2024; 15 (1): 7209

  Abstract

  High-fidelity patterning of thin metal films on arbitrary soft substrates promises integrated circuits and devices that can significantly augment the morphological functionalities of freeform electronics. However, existing patterning methods that decisively rely on prefabricated rigid masks are severely incompatible with myriad surfaces. Here, we report printable, stretchable metal-vapor-desorption layers (s-MVDLs) that can enable high-fidelity patterning of thin metal films on freeform polymeric surfaces. The printed rubbery matrix with highly mobile chains effectively repels various metal vapors from the surface and inhibits their condensation, thereby allowing selective metal deposition. The s-MVDLs are printed by direct ink writing techniques, enabling customizable and scalable thin metal patterns ranging from the micrometer to millimeter scale with high fidelity. Furthermore, the superior stretchability and mechanical robustness of the s-MVDLs allow highly compliant deformation along the substrates, enabling the construction of unconventional circuits and devices on multi-curvature, non-developable, and stretchable surfaces.

  View details for DOI 10.1038/s41467-024-51585-2

  View details for PubMedID 39174549

• Shape-memory-assisted self-healing of macroscopic punctures via high-energy-density periodic dynamic polymers with tunable actuation temperature MATTER Shi, Y., Cooper, C. B., Nogusa, T., Lai, J., Lyu, H., Khatib, M., Xu, C., Michalek, L., Bao, Z. 2024; 7 (6)

  View details for DOI 10.1016/j.matt.2024.03.013

  View details for Web of Science ID 001259507400001

• Tuning polymer-backbone coplanarity and conformational order to achieve high-performance printed all-polymer solar cells. Nature communications Wu, Y., Yuan, Y., Sorbelli, D., Cheng, C., Michalek, L., Cheng, H. W., Jindal, V., Zhang, S., LeCroy, G., Gomez, E. D., Milner, S. T., Salleo, A., Galli, G., Asbury, J. B., Toney, M. F., Bao, Z. 2024; 15 (1): 2170

  Abstract

  All-polymer solar cells (all-PSCs) offer improved morphological and mechanical stability compared with those containing small-molecule-acceptors (SMAs). They can be processed with a broader range of conditions, making them desirable for printing techniques. In this study, we report a high-performance polymer acceptor design based on bithiazole linker (PY-BTz) that are on par with SMAs. We demonstrate that bithiazole induces a more coplanar and ordered conformation compared to bithiophene due to the synergistic effect of non-covalent backbone planarization and reduced steric encumbrances. As a result, PY-BTz shows a significantly higher efficiency of 16.4% in comparison to the polymer acceptors based on commonly used thiophene-based linkers (i.e., PY-2T, 9.8%). Detailed analyses reveal that this improvement is associated with enhanced conjugation along the backbone and closer interchain π-stacking, resulting in higher charge mobilities, suppressed charge recombination, and reduced energetic disorder. Remarkably, an efficiency of 14.7% is realized for all-PSCs that are solution-sheared in ambient conditions, which is among the highest for devices prepared under conditions relevant to scalable printing techniques. This work uncovers a strategy for promoting backbone conjugation and planarization in emerging polymer acceptors that can lead to superior all-PSCs.

  View details for DOI 10.1038/s41467-024-46493-4

  View details for PubMedID 38461153

  View details for PubMedCentralID 8440764

• Tuning the Mobility of Indacenodithiophene-Based Conjugated Polymers via Coplanar Backbone Engineering CHEMISTRY OF MATERIALS Ji, X., Cheng, H., Schuster, N. J., LeCroy, G. S., Zhang, S., Wu, Y., Michalek, L., Nguyen, B. T., Chiong, J. A., Schrock, M., Tomo, Y., Rech, J., Salleo, A., Gam, S., Lee, G., Tok, J., Bao, Z. 2023; 36 (1): 256-265

  View details for DOI 10.1021/acs.chemmater.3c02006

  View details for Web of Science ID 001139519300001

• Sequence-dependent self-assembly of supramolecular nanofibers in periodic dynamic block copolymers JOURNAL OF MATERIALS CHEMISTRY A Phong, J. K., Cooper, C. B., Michalek, L., Lin, Y., Nishio, Y., Shi, Y., Gong, H., Vigil, J. A., Ilavsky, J., Kuzmenko, I., Bao, Z. 2023

  View details for DOI 10.1039/d3ta06695a

  View details for Web of Science ID 001125326700001

• Degradable semiconducting polymers without long-range order for on-demand degradation of transient electronics JOURNAL OF MATERIALS CHEMISTRY C Chiong, J. A., Michalek, L., Pena-Alcantara, A. E., Ji, X., Schuster, N. J., Bao, Z. 2023

  View details for DOI 10.1039/d3tc03079b

  View details for Web of Science ID 001090295600001

• Tunable 1D and 2D Polyacrylonitrile Nanosheet Superstructures. ACS nano Gong, H., Patino, D. U., Ilavsky, J., Kuzmenko, I., Peña-Alcántara, A. E., Zhu, C., Coffey, A. H., Michalek, L., Elabd, A., Gao, X., Chen, S., Xu, C., Yan, H., Jiang, Y., Wang, W., Peng, Y., Zeng, Y., Lyu, H., Moon, H., Bao, Z. 2023

  Abstract

  Carbon superstructures are widely applied in energy and environment-related areas. Among them, the flower-like polyacrylonitrile (PAN)-derived carbon materials have shown great promise due to their high surface area, large pore volume, and improved mass transport. In this work, we report a versatile and straightforward method for synthesizing one-dimensional (1D) nanostructured fibers and two-dimensional (2D) nanostructured thin films based on flower-like PAN chemistry by taking advantage of the nucleation and growth behavior of PAN. The resulting nanofibers and thin films exhibited distinct morphologies with intersecting PAN nanosheets, which formed through rapid nucleation on existing PAN. We further constructed a variety of hierarchical PAN superstructures based on different templates, solvents, and concentrations. These PAN nanosheet superstructures can be readily converted to carbon superstructures. As a demonstration, the nanostructured thin film exhibited a contact angle of ∼180° after surface modification with fluoroalkyl monolayers, which is attributed to high surface roughness enabled by the nanosheet assemblies. This study offers a strategy for the synthesis of nanostructured carbon materials for various applications.

  View details for DOI 10.1021/acsnano.3c05792

  View details for PubMedID 37668312

• Genetically targeted chemical assembly of polymers specifically localized extracellularly to surface membranes of living neurons. Science advances Zhang, A., Loh, K. Y., Kadur, C. S., Michalek, L., Dou, J., Ramakrishnan, C., Bao, Z., Deisseroth, K. 2023; 9 (32): eadi1870

  Abstract

  Multicellular biological systems, particularly living neural networks, exhibit highly complex organization properties that pose difficulties for building cell-specific biocompatible interfaces. We previously developed an approach to genetically program cells to assemble structures that modify electrical properties of neurons in situ, opening up the possibility of building minimally invasive cell-specific structures and interfaces. However, the efficiency and biocompatibility of this approach were challenged by limited membrane targeting of the constructed materials. Here, we design a method for highly localized expression of enzymes targeted to the plasma membrane of primary neurons, with minimal intracellular retention. Next, we show that polymers synthesized in situ by this approach form dense extracellular clusters selectively on the targeted cell membrane and that neurons remain viable after polymerization. Last, we show generalizability of this method across a range of design strategies. This platform can be readily extended to incorporate a broad diversity of materials onto specific cell membranes within tissues and may further enable next-generation biological interfaces.

  View details for DOI 10.1126/sciadv.adi1870

  View details for PubMedID 37556541

• Environmentally stable and stretchable polymer electronics enabled by surface-tethered nanostructured molecular-level protection. Nature nanotechnology Zheng, Y., Michalek, L., Liu, Q., Wu, Y., Kim, H., Sayavong, P., Yu, W., Zhong, D., Zhao, C., Yu, Z., Chiong, J. A., Gong, H., Ji, X., Liu, D., Zhang, S., Prine, N., Zhang, Z., Wang, W., Tok, J. B., Gu, X., Cui, Y., Kang, J., Bao, Z. 2023

  Abstract

  Stretchable polymer semiconductors (PSCs) are essential for soft stretchable electronics. However, their environmental stability remains a longstanding concern. Here we report a surface-tethered stretchable molecular protecting layer to realize stretchable polymer electronics that are stable in direct contact with physiological fluids, containing water, ions and biofluids. This is achieved through the covalent functionalization of fluoroalkyl chains onto a stretchable PSC film surface to form densely packed nanostructures. The nanostructured fluorinated molecular protection layer (FMPL) improves the PSC operational stability over an extended period of 82 days and maintains its protection under mechanical deformation. We attribute the ability of FMPL to block water absorption and diffusion to its hydrophobicity and high fluorination surface density. The protection effect of the FMPL (~6 nm thickness) outperforms various micrometre-thick stretchable polymer encapsulants, leading to a stable PSC charge carrier mobility of ~1 cm2 V-1 s-1 in harsh environments such as in 85-90%-humidity air for 56 days or in water or artificial sweat for 42 days (as a benchmark, the unprotected PSC mobility degraded to 10-6 cm2 V-1 s-1 in the same period). The FMPL also improved the PSC stability against photo-oxidative degradation in air. Overall, we believe that our surface tethering of the nanostructured FMPL is a promising approach to achieve highly environmentally stable and stretchable polymer electronics.

  View details for DOI 10.1038/s41565-023-01418-y

  View details for PubMedID 37322142

• Shear-aligned large-area organic semiconductor crystals through extended pi-pi interaction JOURNAL OF MATERIALS CHEMISTRY C Zhang, S., Talnack, F., Jousselin-Oba, T., Bhat, V., Wu, Y., Lei, Y., Tomo, Y., Gong, H., Michalek, L., Zhong, D., Wu, C., Yassar, A., Mannsfeld, S., Risko, C., Frigoli, M., Bao, Z. 2023

  View details for DOI 10.1039/d3tc01311a

  View details for Web of Science ID 001006838400001

• Autonomous alignment and healing in multilayer soft electronics using immiscible dynamic polymers. Science (New York, N.Y.) Cooper, C. B., Root, S. E., Michalek, L., Wu, S., Lai, J. C., Khatib, M., Oyakhire, S. T., Zhao, R., Qin, J., Bao, Z. 2023; 380 (6648): 935-941

  Abstract

  Self-healing soft electronic and robotic devices can, like human skin, recover autonomously from damage. While current devices use a single type of dynamic polymer for all functional layers to ensure strong interlayer adhesion, this approach requires manual layer alignment. In this study, we used two dynamic polymers, which have immiscible backbones but identical dynamic bonds, to maintain interlayer adhesion while enabling autonomous realignment during healing. These dynamic polymers exhibit a weakly interpenetrating and adhesive interface, whose width is tunable. When multilayered polymer films are misaligned after damage, these structures autonomously realign during healing to minimize interfacial free energy. We fabricated devices with conductive, dielectric, and magnetic particles that functionally heal after damage, enabling thin-film pressure sensors, magnetically assembled soft robots, and underwater circuit assembly.

  View details for DOI 10.1126/science.adh0619

  View details for PubMedID 37262169

• Effect of Molecular Weight on the Morphology of a Polymer Semiconductor-Thermoplastic Elastomer Blend ADVANCED ELECTRONIC MATERIALS Pena-Alcantara, A., Nikzad, S., Michalek, L., Prine, N., Wang, Y., Gong, H., Ponte, E., Schneider, S., Wu, Y., Root, S. E., He, M., Tok, J., Gu, X., Bao, Z. 2023

  View details for DOI 10.1002/aelm.202201055

  View details for Web of Science ID 000915963500001

• Realizing Intrinsically Stretchable Semiconducting Polymer Films by Nontoxic Additives ACS MATERIALS LETTERS Cheng, H., Zhang, S., Michalek, L., Ji, X., Luo, S., Cooper, C. B., Gong, H., Nikzad, S., Chiong, J. A., Wu, Y., Zheng, Y., Liu, Q., Zhong, D., Lei, Y., Tomo, Y., Wei, K., Zhou, D., Tok, J., Bao, Z. 2022; 4 (11): 2328-2336

  View details for DOI 10.1021/acsmaterialslett.2c00749

  View details for Web of Science ID 000898404900001

• Photostationary State in Dynamic Covalent Networks ACS MACRO LETTERS Chambers, L. C., Barner-Kowollik, C., Barner, L., Michalek, L., Frisch, H. 2022; 11 (4): 532-536

  Abstract

  We explore a cross-linked polymer network based on a visible light photodynamic [2 + 2] cycloaddition driven by styrylpyrene chemistry. Based on a polymer backbone with pendent styrylpyrene units, the network can be formed by using λ = 450 nm irradiation. Upon irradiation with λ = 340 nm, a photostationary state is generated within the network with ∼17% of the styrylpyrene units open compared to close to 2% in the visible light cured state. The limited fraction of open [2 + 2] couples is caused by their proximity and is in sharp contrast to solution experiments on the photoreactive moiety. Thus, the polymer network retains its mechanical properties even at the photostationary point. We hypothesize that the application of an additional stimulus could serve as a second gate for inducing network disintegration by spacing the [2 + 2] units during ultraviolet irradiation.

  View details for DOI 10.1021/acsmacrolett.2c00097

  View details for Web of Science ID 000790005700019

  View details for PubMedID 35575324

• A versatile and straightforward process to turn plastics into antibacterial materials POLYMER CHEMISTRY Hadiouch, S., Maresca, M., Gigmes, D., Machado, G., Maurel-Pantel, A., Frik, S., Saunier, J., Deniset-Besseau, A., Yagoubi, N., Michalek, L., Barner-Kowollik, C., Guillaneuf, Y., Lefay, C. 2021; 13 (1): 69-79

  View details for DOI 10.1039/d1py01344k

  View details for Web of Science ID 000724952500001

• A Versatile Light-Triggered Radical-Releasing Surface Coating Technology ADVANCED MATERIALS TECHNOLOGIES Boase, N. B., Michalek, L., Hooker, J. P., Fairfull-Smith, K. E. 2022; 7 (4)

  View details for DOI 10.1002/admt.202100898

  View details for Web of Science ID 000707837600001

• Light-Gated Control of Conformational Changes in Polymer Brushes ADVANCED MATERIALS TECHNOLOGIES Bialas, S., Krappitz, T., Walden, S. L., Kalayci, K., Kodura, D., Frisch, H., MacLeod, J. M., Nelson, A., Michalek, L., Barner-Kowollik, C. 2022; 7 (4)

  View details for DOI 10.1002/admt.202100347

  View details for Web of Science ID 000671534700001