title: 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. 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.
authors.affiliation: Thomas J. Watson Laboratories of Applied Physics, ‡Joint Center for Artificial Photosynthesis, and §Materials and Process Simulation Center, California Institute of Technology , 1200 East California Boulevard, Pasadena, California 91125, United States.
authors.forename: Ana M
authors.initials: AM
authors.lastname: Brown
authors.affiliation: Thomas J. Watson Laboratories of Applied Physics, ‡Joint Center for Artificial Photosynthesis, and §Materials and Process Simulation Center, California Institute of Technology , 1200 East California Boulevard, Pasadena, California 91125, United States.
authors.forename: Ravishankar
authors.initials: R
authors.lastname: Sundararaman
authors.affiliation: Thomas J. Watson Laboratories of Applied Physics, ‡Joint Center for Artificial Photosynthesis, and §Materials and Process Simulation Center, California Institute of Technology , 1200 East California Boulevard, Pasadena, California 91125, United States.
authors.forename: Prineha
authors.initials: P
authors.lastname: Narang
authors.affiliation: Thomas J. Watson Laboratories of Applied Physics, ‡Joint Center for Artificial Photosynthesis, and §Materials and Process Simulation Center, California Institute of Technology , 1200 East California Boulevard, Pasadena, California 91125, United States.
authors.forename: William A
authors.initials: WA
authors.lastname: Goddard
authors.affiliation: Thomas J. Watson Laboratories of Applied Physics, ‡Joint Center for Artificial Photosynthesis, and §Materials and Process Simulation Center, California Institute of Technology , 1200 East California Boulevard, Pasadena, California 91125, United States.
authors.forename: Harry A
authors.initials: HA
authors.lastname: Atwater
keywords: density functional theory; dielectric response; hot carriers; resistivity; surface plasmons; transport