The impact of a dopant atom on the distribution of hot electrons and holes in Au-doped Ag nano-clusters

Abstract

The generation of hot carriers (HCs) through the excitation of localized surface plasmon resonance (LSPR) in metal nanostructures is a fascinating phenomenon that fuels both fundamental and applied research. In this study, we employ first principles real-time time-dependent density-functional theory (rt-TDDFT) calculations to elucidate the creation and distribution of HCs within Au-doped Ag nanoclusters: Ag₁₁Cl₃P₇H₂₁, Ag₁₀Au_coreCl₃P₇H₂₁, and Ag₁₀Au_surfCl₃P₇H₂₁ nanoclusters. Our findings indicate that adjustments in HC distribution are achievable through the Au dopant atom, and precise control of HC distribution is possible by manipulating the location of the Au dopant atom. When employing a Gaussian laser pulse tailored to match the LSPR frequency, a substantial accumulation of HCs in the Ag–P bond is observed. This finding suggests a weakening of the Ag–P bonds and, consequently, the initiation of bond stretching. We propose that these findings open up possibilities for tuning HCs in Au-doped chemically functionalized Ag nanoclusters.