Halogen-Doped Chevrel Phase Janus Monolayers for Photocatalytic Water Splitting

Chevrel non-van der Waals crystals are promising candidates for the fabrication of novel 2D materials due to their versatile crystal structure formed by covalently bonded (Mo6X8) clusters (X-chalcogen atom). Here, we present a comprehensive theoretical study of the stability and properties of Mo-based Janus 2D structures with Chevrel structures consisting of chalcogen and halogen atoms via density functional theory calculations. Based on the analysis performed, we determined that the S2Mo3I2 monolayer is the most promising structure for overall photocatalytic water-splitting application due to its appropriate band alignment and its ability to absorb visible light. The modulated Raman spectra for the representative structures can serve as a blueprint for future experimental verification of the proposed structures.