Interfacial Charge Transfer Circumventing Momentum Mismatch at Two-Dimensional van der Waals Heterojunctions.

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Interfacial charge separation and recombination at heterojunctions of monolayer transition metal dichalcogenides (TMDCs) are of interest to two-dimensional optoelectronic technologies. These processes can involve large changes in parallel momentum vector due to the confinement of electrons and holes to the K valleys in each layer. Because these high-momentum valleys are usually not aligned across the interface of two TMDC monolayers, how parallel momentum is conserved in the charge separation or recombination process becomes a key question. Here we probe this question using the model system of a type-II heterojunction formed by MoS2 and WSe2 monolayers and the experimental technique of femtosecond pump-probe spectroscopy. Upon photoexcitation specifically of WSe2 at the heterojunction, we observe ultrafast (<40 fs) electron transfer from WSe2 to MoS2, independent of the angular alignment and thus momentum mismatch between the two TMDCs. The resulting interlayer charge transfer exciton decays via nonradiative recombination with rates varying by up to three-orders of magnitude from sample to sample but with no correlation with interlayer angular alignment. We suggest that the initial interfacial charge separation and the subsequent interfacial charge recombination processes circumvent momentum mismatch via excess electronic energy and via defect-mediated recombination, respectively.