A variety of advanced photonic applications rely on efficient generation of hot carriers within metal nanoparticles and charge transfer to surrounding molecules or materials. This talk will summarize recent progress on controlling/measuring ultrafast electron photoemission dynamics in plasmonic nanostructures, with vignettes sampling the following areas. 1) Scanning photoionization imaging microscopy (SPIM) and angle-resolved velocity map imaging (VMI) methods have been exploited to characterize volume vs. surface contributions to nanoplasmonic hot electron emission from gold nanorods as a function of aspect ratio (from highly prolate to near spherical). 2) Purely isotropic plasmonic nanostructures have been studied, specifically gold nanospheres and nanoshells, which result in surprisingly anistropic hot electron emission distributions that can be continuously controlled via laser polarization. 3) Ultrafast pump-probe VMI studies are used to explore energies and cooling lifetimes for hot electron distributions in well-characterized nanoplasmonic structures. 4) Theoretical models have been developed based on plasmonic electric field distributions within the nanoparticle volume and ballistic Monte Carlo modeling of the hot electron dynamics, that recapitulate the SPIM/VMI experimental results in near quantitative detail. The results demonstrate a remarkably predictive understanding of the underlying physics and possibilities for ultrafast spatiotemporal control over hot carrier dynamics.

Ultrafast optical control over hot electron dynamics in nanoplasmonic systems

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ACS Fall 2022

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