Emma Simmerman

All Publications

• Structural, Electronic, and Optical Properties of Moiré Materials: A Computational Modeling Handbook ANNUAL REVIEW OF MATERIALS RESEARCH Georgaras, J. D., Chen, E., Ramdas, A., Simmerman, E., Shi, Y., Pokawanvit, S., Haber, J. B., Altman, A., Mauri, Z., Wang, A., Kundu, S., Ciccarino, C., da Jornada, F. H. 2026; 56 (1): 25-65

  View details for DOI 10.1146/annurev-matsci-072924-102520

  View details for Web of Science ID 001810064300010

• Giant Plasmon-Exciton Coupling in Small Plasmonic Nanoparticles from an Ab Initio GW-BSE Approach. Nano letters Simmerman, E. M., Altman, A. R., da Jornada, F. H. 2026

  Abstract

  Plasmonic nanocatalysts have emerged as highly tunable photocatalytic systems for driving nonequilibrium chemistry. However, the underlying microscopic mechanisms are poorly understood, since prevailing models wash out many-body interactions or atomistic details. Here, we address this gap by studying a prototypical small plasmonic nanoparticle within a first-principles GW plus Bethe-Salpeter equation approach. Despite their metallic composition, we find that electronic correlations qualitatively change the electronic and optical properties of this system. The optical response is dominated by plexcitons─plasmons hybridized with strongly bound (>2 eV) electron-hole pairs─showing that the established understanding of nanoparticles underpinned by free electron models is qualitatively incorrect for small nanoparticles. Additionally, we develop a quantitative metric of plasmonicity based on the excited-state wavefunctions and find that one dopant atom perturbs both the low-energy excitons and plasmonic states. Our results suggest that excitonic effects may influence optically driven chemical reactions in small metallic nanoparticles.

  View details for DOI 10.1021/acs.nanolett.5c05340

  View details for PubMedID 41587340

• Nanoscale and ultrafast <i>in situ</i> techniques to probe plasmon photocatalysis CHEMICAL PHYSICS REVIEWS Carlin, C. C., Dai, A. X., Al-Zubeidi, A., Simmerman, E. M., Oh, H., Gross, N., Lee, S. A., Link, S., Landes, C. F., da Jornada, F. H., Dionne, J. A. 2023; 4 (4)

  View details for DOI 10.1063/5.0163354

  View details for Web of Science ID 001112242700001

• Controlling Valley-Specific Light Emission from Monolayer MoS2 with Achiral Dielectric Metasurfaces. Nano letters Liu, Y., Lau, S. C., Cheng, W., Johnson, A., Li, Q., Simmerman, E., Karni, O., Hu, J., Liu, F., Brongersma, M. L., Heinz, T. F., Dionne, J. A. 2023

  Abstract

  Excitons in two-dimensional transition metal dichalcogenides have a valley degree of freedom that can be optically manipulated for quantum information processing. Here, we integrate MoS2 monolayers with achiral silicon disk array metasurfaces to enhance and control valley-specific absorption and emission. Through the coupling to the metasurface electric and magnetic Mie modes, the intensity and lifetime of the emission of neutral excitons, trions, and defect bound excitons can be enhanced and shortened, respectively, while the spectral shape can be modified. Additionally, the degree of polarization (DOP) of exciton and trion emission from the valley can be symmetrically enhanced at 100 K. The DOP increase is attributed to both the metasurface-enhanced chiral absorption of light and the metasurface-enhanced exciton emission from the Purcell effect. Combining Si-compatible photonic design with large-scale 2D materials integration, our work makes an important step toward on-chip valleytronic applications approaching room-temperature operation.

  View details for DOI 10.1021/acs.nanolett.3c01630

  View details for PubMedID 37347949

• Characterizing dark state kinetics and single molecule fluorescence of FusionRed and FusionRed-MQ at low irradiances. Physical chemistry chemical physics : PCCP Mukherjee, S., Thomas, C., Wilson, R., Simmerman, E., Hung, S., Jimenez, R. 2022

  Abstract

  The presence of dark states causes fluorescence intermittency of single molecules due to transitions between "on" and "off" states. Genetically encodable markers such as fluorescent proteins (FPs) exhibit dark states that make several super-resolved single-molecule localization microscopy (SMLM) methods possible. However, studies quantifying the timescales and nature of dark state behavior for commonly used FPs under conditions typical of widefield and total internal reflection fluorescence (TIRF) microscopy remain scarce and pre-date many new SMLM techniques. FusionRed is a relatively bright red FP exhibiting fluorescence intermittency and has thus been identified as a potential candidate for SMLM. We herein characterize the rates for dark-state conversion and the subsequent ground-state recovery of FusionRed and its 2.5-fold brighter descendent FusionRed L175M M42Q (FusionRed-MQ) at low irradiances (1-10 W cm-2), which were previously unexplored experimental conditions. We characterized the kinetics of dark state transitions in these two FPs by using single molecule blinking and ensemble photobleaching experiments bridged with a dark state kinetic model. We find that at low irradiances, the recovery process to the ground state is minimally light-driven and FusionRed-MQ has a 1.3-fold longer ground state recovery time indicating a conformationally restricted dark-state chromophore in comparison to FusionRed. Our studies indicate that the brighter FusionRed-MQ variant exhibits higher dark state conversion rates with longer ground state recovery lifetimes, thus it is potentially a better candidate for SMLM applications than its progenitor FusionRed.

  View details for DOI 10.1039/d2cp00889k

  View details for PubMedID 35642612

• Reconfigurable Quantum Local Area Network Over Deployed Fiber PRX QUANTUM Alshowkan, M., Williams, B. P., Evans, P. G., Rao, N. S., Simmerman, E. M., Lu, H., Lingaraju, N. B., Weiner, A. M., Marvinney, C. E., Pai, Y., Lawrie, B. J., Peters, N. A., Lukens, J. M. 2021; 2 (4)

  View details for DOI 10.1103/PRXQuantum.2.040304

  View details for Web of Science ID 000705671400001

• A Reconfigurable Quantum Local Area Network Over Deployed Fiber Alshowkan, M., Williams, B. P., Evans, P. G., Rao, N. S., Simmerman, E. M., Lu, H., Lingaraju, N. B., Weiner, A. M., Peters, N. A., Lukens, J. M., IEEE IEEE. 2021

  View details for Web of Science ID 000831479800387

• Remote State Preparation in a Reconfigurable Quantum Local Area Network Alshowkan, M., Williams, B. P., Evans, P. G., Rao, N. S., Simmerman, E. M., Lingaraju, N. B., Lu, H., Weiner, A. M., Marvinney, C. E., Pai, Y., Lawrie, B. J., Peters, N. A., Lukens, J. M., IEEE IEEE. 2021

  View details for DOI 10.1109/IPC48725.2021.9593052

  View details for Web of Science ID 000866488100210

• Fully Arbitrary Control of Frequency-Bin Qubits PHYSICAL REVIEW LETTERS Lu, H., Simmerman, E. M., Lougovski, P., Weiner, A. M., Lukens, J. M. 2020; 125 (12): 120503

  Abstract

  Accurate control of two-level systems is a longstanding problem in quantum mechanics. One such quantum system is the frequency-bin qubit: a single photon existing in superposition of two discrete frequency modes. In this Letter, we demonstrate fully arbitrary control of frequency-bin qubits in a quantum frequency processor for the first time. We numerically establish optimal settings for multiple configurations of electro-optic phase modulators and pulse shapers, experimentally confirming near-unity mode-transformation fidelity for all fundamental rotations. Performance at the single-photon level is validated through the rotation of a single frequency-bin qubit to 41 points spread over the entire Bloch sphere, as well as tracking of the state path followed by the output of a tunable frequency beam splitter, with Bayesian tomography confirming state fidelities F_{ρ}>0.98 for all cases. Such high-fidelity transformations expand the practical potential of frequency encoding in quantum communications, offering exceptional precision and low noise in general qubit manipulation.

  View details for DOI 10.1103/PhysRevLett.125.120503

  View details for Web of Science ID 000568998900003

  View details for PubMedID 33016737

• Efficient compressive and Bayesian characterization of biphoton frequency spectra OPTICS LETTERS Simmerman, E. M., Lu, H., Weiner, A. M., Lukens, J. M. 2020; 45 (10): 2886-2889

  Abstract

  Frequency-bin qudits constitute a promising tool for quantum information processing, but their high dimensionality can make for tedious characterization measurements. Here we introduce and compare compressive sensing and Bayesian mean estimation for recovering the spectral correlations of entangled photon pairs. Using a conventional compressive sensing algorithm, we reconstruct joint spectra with up to a 26-fold reduction in measurement time compared to the equivalent raster scan. Applying a custom Bayesian model to the same data, we then additionally realize reliable and consistent quantification of uncertainty. These efficient methods of biphoton characterization should advance our ability to use the high degree of parallelism and complexity afforded by frequency-bin encoding.

  View details for DOI 10.1364/OL.392694

  View details for Web of Science ID 000535920600052

  View details for PubMedID 32412493