The effects of intercalated environmental gas molecules on carrier dynamics in WSe₂/WS₂ heterostructures

Effective tuning of carrier dynamics in two-dimensional (2D) materials is significant for multi-scene device applications. Using first-principles and ab initio nonadiabatic molecular dynamics calculations, the kinetics of O₂, H₂O, and N₂ intercalation into 2D WSe₂/WS₂ van der Waals heterostructures and its effect on carrier dynamics have been comprehensively explored. It is found that the O₂ molecule prefers to dissociate into atomic O atoms spontaneously after intercalation of WSe₂/WS₂ heterostructures, whereas H₂O and N₂ molecules remain intact. O₂ intercalation significantly speeds up the electron separation process, while H₂O intercalation largely speeds up the hole separation process. The lifetime of excited carriers can be prolonged by O₂ or H₂O or N₂ intercalations. These intriguing phenomena can be attributed to the effect of interlayer coupling, and the underlying physical mechanism for tuning the carrier dynamics is fully discussed. Our results provide useful guidance for the experimental design of 2D heterostructures for optoelectronic applications in photocatalysts and solar energy cells.