Transport of hot carriers in plasmonic nanostructures

Abstract

Plasmonic hot carrier devices extract excited carriers from metal nanostructures before equilibration, and have the potential to surpass semiconductor light absorbers. However their efficiencies have so far remained well below theoretical limits, which necessitates quantitative prediction of carrier transport and energy loss in plasmonic structures to identify and overcome bottlenecks in carrier harvesting. 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 at length scales ranging from tens to several hundreds of nanometers, enabling first-principles design of hot carrier devices.

10 pages, 5 figures

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• Non-Equilibrium Phonon Transport Across Nanoscale Interfaces
• Energy-Resolved Femtosecond Hot Electron Dynamics in Single Plasmonic Nanoparticles
• Theory of Non-equilibrium "Hot" Carriers in Direct Band-gap Semiconductors Under Continuous Illumination
• Nonlinear photoluminescence in gold thin films
• On-chip Single-crystal Plasmonic Optoelectronics for Efficient Hot Carrier Collection and Photovoltage Detection
• Accelerating analysis of Boltzmann equations using Gaussian mixture models: Application to quantum Bose-Fermi mixtures
• Unraveling the temperature dynamics and hot electron generation in tunable gap-plasmon metasurface absorbers