4.8 Article

Energy-Resolved Femtosecond Hot Electron Dynamics in Single Plasmonic Nanoparticles

Journal

ACS NANO
Volume 17, Issue 11, Pages 10721-10732

Publisher

AMER CHEMICAL SOC
DOI: 10.1021/acsnano.3c02062

Keywords

hot electrons; ballistic dynamics; angle-resolved; photoemission spectroscopy; single-particle; Monte Carlo; Boltzmann theory

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We investigated the effects of nanoscale structure on the femtosecond dynamics of gold nanoparticles using time-, angle-, and energy-resolved photoemission spectroscopy. We found that nanoparticles as small as 10 nm serve as excellent platforms for studying intrinsic metal dynamics.
Efficientexcitation and harvesting of hot carriers from nanoscalemetals is central to many emerging photochemical, photovoltaic, andultrafast optoelectronic applications. Nevertheless, direct experimentalevidence of the energy-dependent femtosecond dynamics in ubiquitoustens-of-nanometer gold structures remains elusive, despite the potentiallyrich interplay between interfacial and internal plasmonic fields,excitation distributions, and scattering processes. To explore theeffects of nanoscale structure on these dynamics, we employ simultaneoustime-, angle-, and energy-resolved photoemission spectroscopy of singleplasmonic nanoparticles. Photoelectron velocity and electric fielddistributions reveal bulk-like ballistic hot electron transport indifferent geometries, lacking any signatures of surface effects. Energy-resolveddynamics are measured in the 1-2 eV range and extrapolatedto lower energies via Boltzmann theory, providing a detailed viewof hot electron lifetimes within nanoscale gold. We find that particleswith relevant dimensions as small as 10 nm serve as exemplary platformsfor studying intrinsic metal dynamics.

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