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Photo-induced charge separation in transition metal dichalcogenideheterobilayers is being explored for moir\'e excitons, spin-valleypolarization, and quantum phases of excitons/electrons. While differentmomentum spaces may be critically involved in charge separation dynamics,little is known directly from experiments. Here we determine momentum-resolvedelectron dynamics in the WS2/MoS2 heterobilayer using time and angle resolvedphotoemission 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. Theinterlayer charge transfer is accompanied by momentum-specific bandrenormalization. These findings reveal the essential role of phonon scattering,the coexistence of direct and indirect interlayer excitons, and constraints onspin-valley polarization.

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