Exploring plasmonic effect on exciton transport: A theoretical insight from macroscopic quantum electrodynamics.

Abstract

Exciton transport in extended molecular systems and how to manipulate such transport in a complex environment are essential to many energy and optical-related applications. We investigate the mechanism of plasmon-coupled exciton transport by using the Pauli master equation approach, combined with kinetic rates derived from macroscopic quantum electrodynamics. Through our theoretical framework, we demonstrate that the presence of a silver nanorod induces significant frequency dependence in the ability of transporting exciton through a molecule chain, indicated by the exciton diffusion coefficient, due to the dispersive nature of the silver dielectric response. Compared with the same system in vacuum, great enhancement (up to a factor of 103) in the diffusion coefficient can be achieved by coupling the resonance energy transfer process to localized surface plasmon polariton modes of the nanorod. Furthermore, our analysis reveals that the diffusion coefficients with the nearest-neighbor coupling approximation are ∼10 times smaller than the results obtained beyond this approximation, emphasizing the significance of long-range coupling in exciton transport influenced by plasmonic nanostructures. This study not only paves the way for exploring practical approaches to study plasmon-coupled exciton transport but also provides crucial insights for the design of innovative plasmon-assisted photovoltaic applications.