Single-Atom Dopants in Plasmonic Nanocatalysts
Daniel Sorvisto, Patrick Rinke, Tuomas Rossi
Abstract
High Resolution Image Download MS PowerPoint Slide Bimetallic nanostructures combining plasmonic and catalytic metals are promising for tailoring and enhancing plasmonic hot-carrier generation utilized in plasmonic catalysis. In this work, we study the plasmonic hot-carrier generation in noble metal nanoparticles (Ag, Au, and Cu) with single-atom dopants (Ag, Au, Cu, Pd, and Pt) with first-principles time-dependent density functional theory calculations. Our results show that the local hot-carrier generation at the dopant atom is greatly altered by the dopant element while the plasmonic response of the nanoparticle as a whole is not significantly affected. In particular, hot holes at the dopant atom originate from the discrete d-electron states of the dopant, and the energies of these d-electron states and hence those of the hot holes depend on the dopant element, which opens up the possibility to tune hot-carrier generation with suitable dopants.