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

Brown, Ana M.; Sundararaman, Ravishankar; Narang, Prineha; Goddard, William A.; Atwater, Harry A.

doi:10.1021/acsnano.5b06199

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

Journal Article · Thu Dec 10 00:00:00 EST 2015 · ACS Nano

DOI:https://doi.org/10.1021/acsnano.5b06199· OSTI ID:1371056

Brown, Ana M. ^[1]; Sundararaman, Ravishankar ^[1]; Narang, Prineha ^[1]; Goddard, William A. ^[1]; Atwater, Harry A. ^[1]

California Inst. of Technology (CalTech), Pasadena, CA (United States)

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.

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Research Organization:: Energy Frontier Research Centers (EFRC) (United States). Light-Material Interactions in Energy Conversion (LMI)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); National Science Foundation (NSF)

Grant/Contract Number:: SC0001293; SC0004993; AC02-05CH11231

OSTI ID:: 1371056

Journal Information:: ACS Nano, Vol. 10, Issue 1; Related Information: LMI partners with California Institute of Technology (lead); Harvard University; University of Illinois, Urbana-Champaign; Lawrence Berkeley National Laboratory; ISSN 1936-0851

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 469 works

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Journal Article · Wed Dec 23 00:00:00 EST 2009 · Phys. Rev. B · OSTI ID:1371056

Jablan, Marinko; Buljan, Hrvoje; Soljacic, Marin

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36 MATERIALS SCIENCE
surface plasmons
hot carriers
transport
resistivity
dielectric response
density functional theory

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

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