Enhanced electron–phonon coupling by delocalizing phonon states for desirable interlayer transfer of excited charges in MoSSe/WS2 heterobilayer.

Regulating the interlayer transfer of excited charges is challenging but crucial for high-efficiency photoelectric conversion devices based on semiconductor heterojunction. In this work, the interlayer transfer and recombination of excited charges are investigated for the heterobilayers based on monolayer MoSSe and WS2 by combining density functional theory calculation with nonadiabatic molecular dynamics simulation. Our results reveal that the heterobilayers possess type-II band alignments and the interface engineering from S–Se to S–S stacking configuration reverses the spatial distribution of valence and conduction bands from MoSSe and WS2 to WS2 and MoSSe layers, respectively, which produces interlayer transfer of excited charges in opposite direction. The interface engineering also causes the delocalization of out-of-plane phonon states from the WS2 layer to both WS2 and MoSSe layers. This delocalized character in S–S configuration facilitates the simultaneous coupling of out-of-plane phonon states with the localized donor and acceptor electronic states, accelerates the motion of interface atoms, and reduces the band energy differences, which synergistically promote interlayer transfer of excited charges. As a result, the interlayer transfer of excited charges in S–S configuration is faster than that in S–Se configuration. Our investigation demonstrates that delocalizing phonon states through interface engineering can regulate electron–phonon coupling and interlayer transfer of excited charges. [ABSTRACT FROM AUTHOR]