Janus MoXY (X/Y = S, Se, Te) monolayers for photocatalytic water splitting: Performance investigation and regulation via first-principles and nonadiabatic molecular dynamics.

In this study, taking MoXY (X/Y = S, Se, Te) monolayers as an example, we systematically investigate the regulatory role of the polarization induced by elemental variation in the properties of low-dimensional materials, using first-principles calculations combined with nonadiabatic molecular dynamics (NAMD) simulations. The polarization can significantly affect the band edge positions and photocatalytic performance of asymmetric MoXY and effectively lower the reaction energy barriers, thus facilitating photocatalytic water-splitting. In terms of NAMD, this polarization can alter nonadiabatic coupling strength and govern excited-state carrier properties. In addition, the effects of temperature and electron-phonon coupling on the carrier lifetime of the system are also taken into account in this study. This study provides a new theoretical perspective for the selection of photocatalytic materials and offers valuable insights into investigating the manipulation of carrier dynamics in two-dimensional materials.