Unique Hot Carrier Distributions from Scattering-Mediated Absorption

Light-initiated generation of energetic carriers has attracted attention as a paradigm for photocatalysis and solar energy conversion, and the use of noble metal nanoparticles that support LSPR has been widely explored as a medium for realizing this paradigm. It was recently shown that composite nanostructures enabling the interplay between dielectric scattering resonances and broadband absorption in small metal nanostructures, a phenomenon termed scattering-mediated absorption (SMA), can be used to mediate energetic carrier transfer and selective photochemistry with low-intensity light. We will present results from a multiscale modeling approach for elucidating the hot carrier dynamics initiated by SMA. Our calculations reveal that unique hot carrier distributions and dynamics arise from SMA compared to plasmon excitation, and suggest that it may lead to more efficient hot carrier generation than plasmon resonance under the same external illumination conditions. These results are instrumental in understanding the phenomena of scattering-mediated hot carrier generation, which has potential for expanding the palette of materials that can be utilized for hot carrier mediated photochemistry beyond plasmonic metals and for enabling unique pathways for photocatalytic transformations.