Enhancement of valley polarization at high photoexcited densities in MoS2 monolayers

Abstract: We have investigated the steady-sate valley polarization and valley coherence of encapsulated MoS2 monolayer as a function of the temperature and the power density with a continuous wave laser excitation. Both valley polarization and coherence exhibit a non-monotonic dependence on sample temperature, attaining a local maximum at T=40 K. This has been recently attributed to a motional narrowing effect: an enhancement of the valley relaxation time occurs when the scattering rate increases. At a fixed temperature of T=6 K, a two-fold increase of the steady-state valley polarization is achieved by increasing the laser excitation power, which we attribute to a local heating induced by the energy relaxation of photoexcited excitons outside the light cone and to an increase in the exciton-exciton scattering rate. In contrast, in the same power range only a moderate enhancement of valley coherence is observed. Further increasing the excitation power leads to a small reduction of valley polarization but a dramatic loss of valley coherence. Supported by spatial imaging of the excitonic luminescence and polarization, we attribute this behaviour to the detrimental role of exciton-exciton interactions on the pure dephasing rate.