title: Theoretical predictions for hot-carrier generation from surface plasmon decay.
abstract: Decay of surface plasmons to hot carriers finds a wide variety of applications in energy conversion, photocatalysis and photodetection. However, a detailed theoretical description of plasmonic hot-carrier generation in real materials has remained incomplete. Here we report predictions for the prompt distributions of excited 'hot' electrons and holes generated by plasmon decay, before inelastic relaxation, using a quantized plasmon model with detailed electronic structure. We find that carrier energy distributions are sensitive to the electronic band structure of the metal: gold and copper produce holes hotter than electrons by 1-2 eV, while silver and aluminium distribute energies more equitably between electrons and holes. Momentum-direction distributions for hot carriers are anisotropic, dominated by the plasmon polarization for aluminium and by the crystal orientation for noble metals. We show that in thin metallic films intraband transitions can alter the carrier distributions, producing hotter electrons in gold, but interband transitions remain dominant.
authors.affiliation: Joint Center for Artificial Photosynthesis, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA.
authors.forename: Ravishankar
authors.initials: R
authors.lastname: Sundararaman
authors.affiliation: 1] Joint Center for Artificial Photosynthesis, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA [2] Thomas J. Watson Laboratories of Applied Physics, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA.
authors.forename: Prineha
authors.initials: P
authors.lastname: Narang
authors.affiliation: 1] Joint Center for Artificial Photosynthesis, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA [2] Division of Physics, Mathematics and Astronomy, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA.
authors.forename: Adam S
authors.initials: AS
authors.lastname: Jermyn
authors.affiliation: 1] Joint Center for Artificial Photosynthesis, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA [2] Materials and Process Simulation Center, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA.
authors.forename: William A
authors.initials: WA
authors.lastname: Goddard
authors.affiliation: 1] Joint Center for Artificial Photosynthesis, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA [2] Thomas J. Watson Laboratories of Applied Physics, California Institute of Technology, 1200 East California Boulevard, Pasadena, California 91125, USA.
authors.forename: Harry A
authors.initials: HA
authors.lastname: Atwater