Theory of Plasmonic Hot-Carrier Generation and Relaxation

Zhang, Yu

doi:10.1021/acs.jpca.1c05837

Theory of Plasmonic Hot-Carrier Generation and Relaxation

Journal Article · Fri Oct 08 00:00:00 EDT 2021 · Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory

DOI:https://doi.org/10.1021/acs.jpca.1c05837· OSTI ID:1826522

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Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Hot-carrier (HC) generation from (localized) surface plasmon decay has recently attracted much attention due to its promising applications in physical, chemical, materials, and energy science. However, the detailed mechanisms of plasmonic HC generation, relaxation, and trapping are less studied. In this work, we developed and applied a quantum-mechanical model and coupled master equation method to study the generation of HCs from plasmon decay and their following relaxation processes with different mechanisms treated on equal footing. First, a quantum-mechanical model for HC generation is developed. Its connection to existing semiclassical models and time-dependent density functional theory (TDDFT) is discussed. Second, the relaxation and lifetimes of HCs are investigated in the presence of electron–electron and electron–phonon interactions. A GW-like approximation is introduced to account for the electron–electron scattering. The numerical simulations on the Jellium nanoparticles with a size up to 1.6 nm demonstrate the electron–electron scattering and electron–phonon scattering dominate different time scale in the relaxation dynamics. We also generalize the model to study the extraction of HCs to attached molecules. The quantum yield of extracting HCs for other applications is found to be size-dependent. In general, the smaller size of NP improves the quantum yield, which is in agreement with recent experimental measurements. Even though we demonstrate this newly developed theoretical formalism with Jellium model, the theory applies to any other atomistic models.

View Accepted Manuscript (DOE)

Research Organization:: Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Laboratory Directed Research and Development (LDRD) Program

Grant/Contract Number:: 89233218CNA000001

OSTI ID:: 1826522

Report Number(s):: LA-UR--21-26367

Journal Information:: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory, Journal Name: Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory Journal Issue: 41 Vol. 125; ISSN 1089-5639

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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Theory of Plasmonic Hot-Carrier Generation and Relaxation

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