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Plasmonic hot carrier devices extract excited carriers from metalnanostructures before equilibration, and have the potential to surpasssemiconductor light absorbers. However their efficiencies have so far remainedwell below theoretical limits, which necessitates quantitative prediction ofcarrier transport and energy loss in plasmonic structures to identify andovercome bottlenecks in carrier harvesting. Here, we present a theoretical andcomputational framework, Non-Equilibrium Scattering in Space and Energy(NESSE), to predict the spatial evolution of carrier energy distributions thatcombines the best features of phase-space (Boltzmann) and particle-based (MonteCarlo) methods. Within the NESSE framework, we bridge first-principleselectronic structure predictions of plasmon decay and carrier collisionintegrals at the atomic scale, with electromagnetic field simulations at thenano- to mesoscale. Finally, we apply NESSE to predict spatially-resolvedenergy distributions of photo-excited carriers that impact the surface ofexperimentally realizable plasmonic nanostructures at length scales rangingfrom tens to several hundreds of nanometers, enabling first-principles designof hot carrier devices.

Transport of hot carriers in plasmonic nanostructures