Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry
Abstract
The behavior of metals across a broad frequency range from microwave to ultraviolet frequencies is of interest in plasmonics, nanophotonics, and metamaterials. Depending on the frequency, losses of collective excitations in metals can be predominantly classical resistive effects or Landau damping. In this context, we present first-principles calculations that capture all of the significant microscopic mechanisms underlying surface plasmon decay and predict the initial excited carrier distributions so generated. Particularly, we include ab initio predictions of phonon-assisted optical excitations in metals, which are critical to bridging the frequency range between resistive losses at low frequencies and direct interband transitions at high frequencies. In the commonly used plasmonic materials, gold, silver, copper, and aluminum, we find that resistive losses compete with phonon-assisted carrier generation below the interband threshold, but hot carrier generation via direct transitions dominates above threshold. Furthermore, we predict energy-dependent lifetimes and mean free paths of hot carriers, accounting for electron–electron and electron–phonon scattering, to provide insight toward transport of plasmonically generated carriers at the nanoscale.
- Authors:
-
- California Inst. of Technology (CalTech), Pasadena, CA (United States)
- Publication Date:
- Research Org.:
- Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)
- OSTI Identifier:
- 1371056
- Grant/Contract Number:
- SC0001293; SC0004993; AC02-05CH11231
- Resource Type:
- Accepted Manuscript
- Journal Name:
- ACS Nano
- Additional Journal Information:
- Journal Volume: 10; Journal Issue: 1; Related Information: LMI partners with California Institute of Technology (lead); Harvard University; University of Illinois, Urbana-Champaign; Lawrence Berkeley National Laboratory; Journal ID: ISSN 1936-0851
- Publisher:
- American Chemical Society (ACS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; surface plasmons; hot carriers; transport; resistivity; dielectric response; density functional theory
Citation Formats
Brown, Ana M., Sundararaman, Ravishankar, Narang, Prineha, Goddard, William A., and Atwater, Harry A. Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry. United States: N. p., 2015.
Web. doi:10.1021/acsnano.5b06199.
Brown, Ana M., Sundararaman, Ravishankar, Narang, Prineha, Goddard, William A., & Atwater, Harry A. Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry. United States. https://doi.org/10.1021/acsnano.5b06199
Brown, Ana M., Sundararaman, Ravishankar, Narang, Prineha, Goddard, William A., and Atwater, Harry A. Thu .
"Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry". United States. https://doi.org/10.1021/acsnano.5b06199. https://www.osti.gov/servlets/purl/1371056.
@article{osti_1371056,
title = {Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry},
author = {Brown, Ana M. and Sundararaman, Ravishankar and Narang, Prineha and Goddard, William A. and Atwater, Harry A.},
abstractNote = {The behavior of metals across a broad frequency range from microwave to ultraviolet frequencies is of interest in plasmonics, nanophotonics, and metamaterials. Depending on the frequency, losses of collective excitations in metals can be predominantly classical resistive effects or Landau damping. In this context, we present first-principles calculations that capture all of the significant microscopic mechanisms underlying surface plasmon decay and predict the initial excited carrier distributions so generated. Particularly, we include ab initio predictions of phonon-assisted optical excitations in metals, which are critical to bridging the frequency range between resistive losses at low frequencies and direct interband transitions at high frequencies. In the commonly used plasmonic materials, gold, silver, copper, and aluminum, we find that resistive losses compete with phonon-assisted carrier generation below the interband threshold, but hot carrier generation via direct transitions dominates above threshold. Furthermore, we predict energy-dependent lifetimes and mean free paths of hot carriers, accounting for electron–electron and electron–phonon scattering, to provide insight toward transport of plasmonically generated carriers at the nanoscale.},
doi = {10.1021/acsnano.5b06199},
journal = {ACS Nano},
number = 1,
volume = 10,
place = {United States},
year = {Thu Dec 10 00:00:00 EST 2015},
month = {Thu Dec 10 00:00:00 EST 2015}
}
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