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Abstract Recent experiments observed significant energy transfer in type-II van der Waals (vdW) heterostructures, such as WS 2 /MoSe 2 , which is surprising due to their staggered band alignment and weak spectral overlap. In this work, we carry out first-principles calculations to shed light on energy and charge transfer in WS 2 /MoSe 2 heterostructure. Incorporating excitonic effect in nonadiabatic electronic dynamics, our first-principles calculations uncover a two-step process in competing energy and charge transfer, unravel their relative efficiencies and explore the means to control their competition. While both Dexter and Förster mechanisms can be responsible for energy transfer, they are shown to operate at different conditions. The excitonic effect is revealed to drive ultrafast energy and charge transfer in type-II WS 2 /MoSe 2 heterostructure. Our work provides a comprehensive picture of exciton dynamics in vdW heterostructures and paves the way for rational design of novel vdW heterostructures for optoelectronic and photovoltaic applications.
Liu et al. (Mon,) studied this question.