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Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry

Brown, Ana M. and Sundararaman, Ravishankar and Narang, Prineha and Goddard, William A., III and Atwater, Harry A. (2016) Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry. ACS Nano, 10 (1). pp. 957-966. ISSN 1936-0851. doi:10.1021/acsnano.5b06199.

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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. Specifically, 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. Finally, 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.

Item Type:Article
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URLURL TypeDescription
Sundararaman, Ravishankar0000-0002-0625-4592
Narang, Prineha0000-0003-3956-4594
Goddard, William A., III0000-0003-0097-5716
Atwater, Harry A.0000-0001-9435-0201
Additional Information:© 2015 American Chemical Society. Received: October 1, 2015; Accepted: December 10, 2015; Publication Date (Web): December 10, 2015. This material is based upon work performed by the Joint Center for Artificial Photosynthesis, a DOE Energy Innovation Hub, supported through the Office of Science of the U.S. Department of Energy under Award Number DE-SC0004993. Calculations in this work used the National Energy Research Scientific Computing Center, a DOE Office of Science User Facility supported by the Office of Science o the U.S. Department of Energy under Contract No. DE-AC02-05CH11231. P.N. is supported by a National Science Foundation Graduate Research Fellowship and by the Resnick Sustainability Institute. A.B. is supported by a National Science Foundation Graduate Research Fellowship, a Link Foundation Energy Fellowship, and the DOE Light−Material Interactions in Energy Conversion Energy Frontier Research Center (DESC0001293). The authors declare no competing financial interest.
Group:Resnick Sustainability Institute, JCAP
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0004993
Department of Energy (DOE)DE-AC02-05CH11231
NSF Graduate Research FellowshipUNSPECIFIED
Resnick Sustainability InstituteUNSPECIFIED
Link FoundationUNSPECIFIED
Department of Energy (DOE)DE-SC0001293
Subject Keywords:surface plasmons, hot carriers, transport, resistivity, dielectric response, density functional theory
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Issue or Number:1
Record Number:CaltechAUTHORS:20160104-150344444
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Official Citation:Nonradiative Plasmon Decay and Hot Carrier Dynamics: Effects of Phonons, Surfaces, and Geometry Ana M. Brown, Ravishankar Sundararaman, Prineha Narang, William A. Goddard, III, and Harry A. Atwater ACS Nano 2016 10 (1), 957-966 DOI: 10.1021/acsnano.5b06199
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:63346
Deposited By: Tony Diaz
Deposited On:04 Jan 2016 23:13
Last Modified:10 Nov 2021 23:15

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