Endowing bilayer transition-metal dichalcogenides (TMDs) with tunable magnetism is significant to investigate the coupling of multiple electron degrees of freedom (DOFs). However, effectively inducing and tuning the magnetic interaction of bilayer TMDs are still challenges. Herein, we report a strategy to tune the interlayer exchange interaction of centimeter-scale MoS₂ bilayer with substitutional doping of Co ion, by introducing sulfur vacancy (V_S) to modulate the interlayer electronic coupling. This strategy could transform the interlayer exchange interaction from antiferromagnetism (AFM) to ferromagnetism (FM), as revealed by the magnetic measurements. Experimental characterizations and theoretical calculations indicate that the enhanced magnetization is mainly because the hybridization of Co 3d band and V_S-induced impurity band alters the forms of interlayer orbital hybridizations between the partial Co atoms in upper and lower layers, and also enhances the intralayer FM. Our work paves the way for tuning the interlayer exchange interaction with defects and could be extended to other two-dimensional (2D) magnetic materials.

Endowing bilayer transition-metal dichalcogenides (TMDs) with tunable magnetism is significant to investigate the coupling of multiple electron degrees of freedom (DOFs). However, effectively inducing and tuning the magnetic interaction of bilayer TMDs are still challenges. Herein, we report a strategy to tune the interlayer exchange interaction of centimeter-scale MoS₂ bilayer with substitutional doping of Co ion, by introducing sulfur vacancy (V_S) 来调制层间电子耦合。正如磁性测量所揭示的那样，该策略可以将层间交换相互作用从反铁磁性（AFM）转变为铁磁性（FM）。实验表征和理论计算表明，增强磁化强度主要是因为 Co 3d 带和 V _S诱导杂质带的杂化改变了上层和下层部分 Co 原子之间的层间轨道杂化形式，也增强了层内 FM . 我们的工作为调整与缺陷的层间交换相互作用铺平了道路，并且可以扩展到其他二维 (2D) 磁性材料。