Stacking pattern effects on the charge carrier dynamics of the MoS2/ BSe heterostructure

The efficiency of electron-hole (e-h) pair separation at the interface of van der Waals (vdW) heterostructures is crucial in determining the solar energy conversion efficiency. In this work, based on the nonadiabatic molecular dynamics (NAMD) simulations, we have studied the photoinduced carrier dynamics of MoS2/BSe, and the effect of stacking configuration is further analyzed. The results demonstrate that the MoS2/BSe heterostructure is consistent with a type-II photogenerated carrier transfer mechanism, with ultrafast interlayer electron and hole transfer time scales of -50 fs and -200 fs, respectively, displaying a weak stacking dependence. Additionally, switching from AA to AB stacking delays the carrier lifetime of the heterostructure by about a factor of two, from 52.14 ns to 98.39 ns, which can be rationalized by the smaller wave function overlap and fast decoherence time of AB stacking. The present offering insights on the development of high-performance solar energy photovoltaic conversion devices on vdW heterostructures.