Interlayer exciton valley polarization dynamics in large magnetic fields

In van der Waals heterostructures consisting of stacked MoSe2 and WSe2 monolayers, optically bright interlayer excitons can be observed when the constituent layers are crystallographically aligned. The symmetry of the monolayers allows for two different types of alignment, in which the momentum-direct interlayer transitions are either valley conserving (R-type alignment) or change the valley index (H-type antialignment). Here, we study the valley polarization dynamics of interlayer excitons in magnetic fields up to 30 T by time-resolved photoluminescence. For all interlayer exciton types, we find a finite initial photoluminescence circular degree of polarization after unpolarized excitation in applied magnetic fields. For interlayer excitons in H-type heterostructures, we observe a systematic increase of the photoluminescence circular degree of polarization with time in applied magnetic fields, which saturates at values close to unity for the largest fields. By contrast, for interlayer excitons in R-type heterostructures, the photoluminescence circular degree of polarization shows a decrease and a zero crossing before saturating with opposite polarization. This unintuitive behavior can be explained by a model considering the different interlayer exciton states in H- and R-type heterostructures and their selection rules coupling photoluminescence helicity and valley polarization.