Hot-carrier generation in plasmonic nanoparticles: Atomic-scale analysis

Metal nanoparticles absorb light much more than their physical size would suggest due to the excitation of a localized surface plasmon resonance. After its excitation, the plasmon resonance decays into high-energy electrons and holes, which, combined with the large absorption cross section, make metal nanoparticles attractive hot-carrier generators for photocatalysis. In this presentation, we describe the femtosecond dynamics of localized surface plasmons in noble metal nanoparticles by using time-dependent density-functional theory (TDDFT). We track the plasmon formation and decay into hot carriers in terms of contributing electron-hole transitions [1,2]. By analyzing the resulting hot-carrier distributions down to atomic-scale detail, we shed light on the hot-carrier generation in catalytically-relevant edge and corner sites of nanoparticles [2].

[1] T. P. Rossi et al., J. Chem. Theory Comput. 13, 4779 (2017).
[2] T. P. Rossi, P. Erhart, and M. Kuisma (unpublished).