Title: Far-from-equilibrium transport of excited carriers in nanostructures,
Abstract: Transport of charged carriers in regimes of strong non-equilibrium is
critical in a wide array of applications ranging from solar energy conversion
and semiconductor devices to quantum information. Plasmonic hot-carrier science
brings this regime of transport physics to the forefront since photo-excited
carriers must be extracted far from equilibrium to harvest their energy
efficiently. Here, we present a theoretical and computational framework,
Non-Equilibrium Scattering in Space and Energy (NESSE), to predict the spatial
evolution of carrier energy distributions that combines the best features of
phase-space (Boltzmann) and particle-based (Monte Carlo) methods. Within the
NESSE framework, we bridge first-principles electronic structure predictions of
plasmon decay and carrier collision integrals at the atomic scale, with
electromagnetic field simulations at the nano- to mesoscale. Finally, we apply
NESSE to predict spatially-resolved energy distributions of photo-excited
carriers that impact the surface of experimentally realizable plasmonic
nanostructures, enabling first-principles design of hot carrier devices.