Ultrafast dynamics in monolayer transition metal dichalcogenides: Interplay of dark excitons, phonons, and intervalley exchange

Artikel i vetenskaplig tidskrift, 2019

Understanding the ultrafast coupling and relaxation mechanisms between valleys in transition metal dichalcogenide semiconductors is of crucial interest for future valleytronic devices. Recent ultrafast pump-probe experiments showed an unintuitive significant bleaching at the excitonic B transition after optical excitation of the energetically lower excitonic A transition. Here, we present a possible microscopic explanation for this surprising effect. It is based on the joint action of exchange coupling and phonon-mediated thermalization into dark exciton states and does not involve a population of the B exciton. Our work demonstrates how intra- and intervalley coupling on a femtosecond timescale governs the optical valley response of 2D semiconductors.