Hot-carrier generation in plasmonic nanoparticles at the atomic scale

Metal nanoparticles support strongly absorbing localized surface plasmon resonances, which render them attractive for plasmon-enhanced hot-carrier generation. Detailed understanding of plasmonic hot-carrier generation at the atomic scale is highly important for plasmonic catalysis as chemical reactions take place at this size scale. In this presentation, we discuss, based on time-dependent density-functional theory modeling, the femtosecond dynamics of plasmon formation and dephasing into hot carriers in metal nanoparticles. Our results suggest that the distribution of hot electrons varies significantly between different atomic sites. In particular, catalytically-relevant surface sites can exhibit enhanced hot-electron generation in comparison to the nanoparticle as a whole [1]. These results indicate possibilities for tailoring hot-carrier distributions by careful design of atomic-scale features in nanoscale systems.

[1] T. P. Rossi et al., ACS Nano 14, 9963 (2020).