Plasmonic nanoparticles are able to break bonds and drive reactions on nearby molecules. The plasmon resonance, thought to play an important role in the catalytic activity, often falls within the visible light region. Hence, plasmonic nanomaterials are a promising new class of catalysts which can operate under benign conditions. However, the mechanisms through which plasmonic nanoparticles activate and/or break the bonds of nearby molecules are still unclear. Herein, we evaluate Ag8-X2 (X = N, H) model systems via real-time time-dependent density functional theory (RT-TDDFT), linear response time-dependent density functional theory (LR-TDDFT), and Ehrenfest dynamics in order to better understand the activation and breakage processes of N2 and H2 facilitated by the presence of the atomic silver wire. We find that dissociation and activation of both small molecules is symmetry- and electric field-dependent, and H2 activates at lower electric field strengths than N2. This study serves as a step towards understanding the time-dependent electron and electron-nuclear dynamics between plasmonic nanowires and small molecules.

Electron and electron-nuclear dynamics of atomic silver nanowire-small molecule systems

ACS Spring Meeting 2021

The official archive and repository for all ACS Meetings & Expositions abstracts and select posters or presentations.