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.