Ultrafast dynamics of spin relaxation in monolayer WSe 2 and the WSe 2 /graphene heterojunction.

Excitonic devices based on two-dimensional (2D) transition metal dichalcogenides (TMDCs) can combine spintronics with valleytronics due to its special energy band structure. In this work, we studied the generation and relaxation processes of spin/valley polarized excitons dynamics in monolayer WSe 2 and its van der Waals (vdW) heterojunction with graphene using a circularly polarized femtosecond pump-probe system. The spin/valley depolarization dynamics of the A exciton in monolayer WSe 2 is found to exhibit a biexponential decay. The fast relaxation process is due to the ultrafast intervalley electron-hole spin-flip exchange coupling and electron-phonon scattering. And the slow relaxation process originates from the recombination and relaxation of the trion states. Graphene has an electron extraction effect on WSe 2 , which prevents the formation of trions. Therefore, the spin/valley depolarization process of the A exciton in the heterojunction exhibits only a fast relaxation process. In both monolayer WSe 2 and its heterojunction with graphene, B/A' excitons exhibit a negative spin/valley polarization which is mainly due to two-photon absorption and excited Bose scattering. Our work systematically studied the spin/valley depolarization dynamics of excitons and revealed possible mechanisms of their differences in isolated 2D WSe 2 and vdW heterojunctions.