Direct measurement of exciton valley coherence in monolayer WSe2

In crystals, energy band extrema in momentum space can be identified by a valley index. The internal quantum degree of freedom associated with valley pseudospin indices can act as a useful information carrier, analogous to electronic charge or spin(1-4). Interest in valleytronics has been revived in recent years following the discovery of atomically thin materials such as graphene and transition metal dichalcogenides(5-7). However, the valley coherence time-a crucial quantity for valley pseudospin manipulation-is difficult to directly probe. In this work, we use two-dimensional coherent spectroscopy to resonantly generate and detect valley coherence of excitons (Coulomb-bound electron-hole pairs) in monolayer WSe2 (refs 8,9). The imposed valley coherence persists for approximately one hundred femtoseconds. We propose that the electron-hole exchange interaction provides an important decoherence mechanism in addition to exciton population recombination. This work provides critical insight into the requirements and strategies for optical manipulation of the valley pseudospin for future valleytronics applications.