Exciton diffusion in MoS2 monolayer from first-principles molecular dynamics

Abstract

First-principles modeling of exciton dynamics coupled with lattice vibrations is important for understanding exciton mobility, which is crucial for various applications. In order to shed light on such coupled exciton–lattice dynamics, in this paper, we use a restricted open-shell Kohn–Sham approach, which is a computationally efficient method for electronic structure calculations in the lowest excited states. Within this framework, we analyze the correlated electron–hole dynamics of a bright exciton in the 1H–MoS2 monolayer in real space at different temperatures and obtain the exciton diffusion rate that is in reasonable agreement with the experimental findings.