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DOE OSTI · 2420367

Ab initio quantum dynamics of plasmonic charge carriers

Li, Wei·Xue, Ting·Mora-Perez, Carlos·Prezhdo, Oleg V.
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Abstract

Surface plasmons respond strongly to electric fields and generate energetic (hot) charge carriers that can be used in optoelectronic devices. However, utilization of hot carriers has to outcompete fast carrier relaxation in metals. Often, the reported efficiencies of nanoscale devices based on plasmon excitations are low and the mechanisms of device operation remain inconsistent within the field. Further developments hinge on fundamental understanding of the nature and kinetics of plasmon decay processes. In this work, we provide an overview of time domain ab initio modeling of hot carrier dynamics, demonstrating that atomistic details of the surface structure of plasmonic materials, and their chemical interaction with semiconducting and molecular charge acceptors and substrates, play key roles in governing the dynamics pathways. Considered case studies represent various dynamics channels and illustrate solar energy and optoelectronic applications.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYcharge transferchemistryhot carriersquantum molecular dynamicssurface plasmon resonancetime-dependent density functional theory

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Li, Wei, Xue, Ting, Mora-Perez, Carlos, Prezhdo, Oleg V.. 2023-03-17. Ab initio quantum dynamics of plasmonic charge carriers. https://doi.org/10.1016/j.trechm.2023.02.010

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