Hot carrier creation in a nanoparticle dimer-molecule composite.

Abstract

Light-matter interactions have garnered considerable interest owing to their burgeoning applications in quantum optics and plasmonics. Utilizing first principles calculations, this work explores the hot carrier (HC) generation and distribution within a composite system made up of a plasmonic nanoparticle dimer and linear polycyclic aromatic hydrocarbon (PAH) molecules. We examine the spatial and energetic distributions of HCs by initiating photoexcitation and allowing localized surface plasmon dephasing. By positioning PAH molecules within the plasmonic nanodimer's gap region, our investigation uncovers HC tuning. Notably, depending on the size of the PAH molecules, there are significant alterations in the HC distribution. Hot electrons (HEs) are distributed across both the nanodimer and the PAH molecule, while hot holes (HHs) become entirely localized on the PAH as the PAH grows larger. These findings improve our understanding of plasmon-molecule coupled states and provide guidance on how to customize HC distributions through the creation of hybrid plasmonic materials.