Tunable Spintronic Structure of Monolayer and Bilayer MoS ₂ Doped With Iron Atom

Doping is a common and effective method for regulating the electronic structure of transition metal dichalcogenides. Based on first‐principles calculations, it is found that the system is effectively transformed into a metal by substituting or adsorbing a typical transition metal element, Fe atom in the monolayer and bilayer MoS 2 structure, respectively, while achieving 100% spin polarization. The key difference is that adsorption is more likely to induce polarization than substitution doping when the same impurity atom is introduced. Additionally, in substitution doping, the coupling between the impurity atom and the intrinsic system is more pronounced. More specifically, the different charge distributions and orbital hybridization in monolayer and bilayer MoS 2 under substitution and adsorption, respectively, cause the system to exhibit half‐metallic characteristics of different spin channels. This discovery has significantly advanced the research and development of the regulatory properties of layered 2D materials similar to graphene.