title: Theory and computation of hot carriers generated by surface plasmon polaritons in noble metals.
abstract: Hot carriers (HC) generated by surface plasmon polaritons (SPPs) in noble metals are promising for application in optoelectronics, plasmonics and renewable energy. However, existing models fail to explain key quantitative details of SPP-to-HC conversion experiments. Here we develop a quantum mechanical framework and apply first-principles calculations to study the energy distribution and scattering processes of HCs generated by SPPs in Au and Ag. We find that the relative positions of the s and d bands of noble metals regulate the energy distribution and mean free path of the HCs, and that the electron-phonon interaction controls HC energy loss and transport. Our results prescribe optimal conditions for HC generation and extraction, and invalidate previously employed free-electron-like models. Our work combines density functional theory, GW and electron-phonon calculations to provide microscopic insight into HC generation and ultrafast dynamics in noble metals.
authors.affiliation: 1] Department of Physics, University of California at Berkeley, 366 LeConte Hall #7300, Berkeley, California 94720, USA [2] Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
authors.forename: Marco
authors.initials: M
authors.lastname: Bernardi
authors.affiliation: 1] Department of Physics, University of California at Berkeley, 366 LeConte Hall #7300, Berkeley, California 94720, USA [2] Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
authors.forename: Jamal
authors.initials: J
authors.lastname: Mustafa
authors.affiliation: 1] Department of Physics, University of California at Berkeley, 366 LeConte Hall #7300, Berkeley, California 94720, USA [2] Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA [3] Molecular Foundry, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA [4] Kavli Institute for Energy Nanosciences at Berkeley, Berkeley, California 94720, USA.
authors.forename: Jeffrey B
authors.initials: JB
authors.lastname: Neaton
authors.affiliation: 1] Department of Physics, University of California at Berkeley, 366 LeConte Hall #7300, Berkeley, California 94720, USA [2] Materials Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720, USA.
authors.forename: Steven G
authors.initials: SG
authors.lastname: Louie