Direct determination of momentum resolved electron transfer in the photo-excited MoS2/WS2 van der Waals heterobilayer by TR-ARPES

Abstract: Photo-induced charge separation in transition metal dichalcogenide heterobilayers is being explored for moir\'e excitons, spin-valley polarization, and quantum phases of excitons/electrons. While different momentum spaces may be critically involved in charge separation dynamics, little is known directly from experiments. Here we determine momentum-resolved electron dynamics in the WS2/MoS2 heterobilayer using time and angle resolved photoemission spectroscopy (TR-ARPES). Upon photoexcitation in the K valleys, we detect electrons in M/2, M, and Q valleys/points on time scales as short as ~70 fs, followed by dynamic equilibration in K and Q valleys in ~400 fs. The interlayer charge transfer is accompanied by momentum-specific band renormalization. These findings reveal the essential role of phonon scattering, the coexistence of direct and indirect interlayer excitons, and constraints on spin-valley polarization.