Unveiling Ultrafast Spin‐Valley Dynamics and Phonon‐Mediated Charge Transfer in MoSe2/WSe2 Heterostructures

Helicity-resolved ultrafast transient absorption spectroscopy is used to study spin-valley polarization dynamics in a vertically stacked MoSe2/WSe2 heterostructure. The experimental findings reveal details of interlayer charge transfer on ultrafast timescales, showing that the spin-valley polarized state of photoexcited carriers is conserved during the charge transfer and formation of interlayer excitons. These results confirm that phonon scattering mediates the interlayer charge transfer process, while a high phonon population at elevated temperatures causes a significant decrease in spin-valley selective charge transfer. Moreover, the experimental findings demonstrate the possibility that interlayer excitons and their spin-valley polarization can be probed in the optical response of intralayer excitons. These findings pave the way for ultrafast detection, control, and manipulation of spin-valley polarized excitons in transition metal dichalcogenide-based 2D heterostructures.