Modulation of the electronic structure of monolayer MoS 2 by main-group metal doping and the mechanism of enhanced photocatalytic performance

Abstract In this work, based on first-principles study, elucidates the regulatory mechanism of IIIA–VA group metal (IIIA: Al, Ga, and In; IVA: Ge, Sn, and Pb; VA: Sb and Bi) doping on the photocatalytic activity of monolayer MoS 2 . Binding energy and molecular dynamics simulations confirm that IIIA–VA group metal elements can be stably anchored at Mo vacancy sites. Such doping introduces holes into the system, induces rearrangement of surface charge, and further leads to the formation of impurity levels within the band gap. It modulates the charge density distribution of the conduction band minimum and valence band maximum across different atoms, and alters the surface electrostatic potential. These changes effectively suppress the recombination of photogenerated carriers, increase the number of catalytic active sites, reduce the work function, thereby facilitating electron transfer and enhancing optical absorption capability. Therefore, IIIA–VA group metal doping serves as an effective strategy for improving the photocatalytic performance of MoS 2 and provides a theoretical foundation for the design of novel and efficient MoS 2 -based photocatalysts.