Quantum-classical modeling of exciton-phonon dynamics in monolayer transition metal dichalcogenides

Monolayer transition metal dichalcogenides (TMDs) exhibit spin-valley polarized excitons with potential optoelectronic and valleytronic applications. Rapid exciton depolarization, however, fundamentally limits their usefulness. While depolarization is known to proceed through a phonon-mediated exchange pathway, the microscopic factors underlying its rapid onset remain unclear. In this talk, I will present our efforts to better understand these factors through reciprocal-space quantum-classical simulations of exciton-phonon scattering. To that end, we combine a detailed material model with a series of truncation parameters that target particular regions of the Brillouin zone. By varying these parameters, we access the infinite size limit and provide detailed insight into the non-Markovian and dynamic interplay of acoustic and optical phonon scattering pathways and exciton dynamics. In doing so, we establish a promising route towards unraveling the microscopic drivers of valley depolarization.