Exciton valley dynamics in monolayer Mo1-xWxSe2 (x = 0, 0.5, 1)

Abstract

We study the exciton valley dynamics in monolayers MoSe2, Mo0.5W0.5Se2, and WSe2 by employing helicity-resolved two-color transient reflection spectroscopy. The valley depolarization dynamics as a function of the excitation laser energy is studied systematically at above-resonant excitation of excitons at 10 K. A longer intervalley scattering time is obtained as the excitation energy approaches the A exciton resonance for the three studied materials. The excitation energy dependence of exciton valley relaxation proves that the long-range electron-hole exchange interaction dominates the intervalley scattering in transition metal dichalcogenide monolayers. The longer valley scattering time and higher valley polarization degree commonly observed for WSe2 than for MoSe2 is discussed to result from the interplay between the intervalley electron-hole exchange interaction and dark-bright exciton scattering, where the existence of energetically lower lying dark excitonic states in monolayer WSe2 favors the suppression of the intervalley electron-hole exchange interaction.