The activation and modulation of the magnetism of MoS2 nanosheets are critical to the development of their application in next-generation spintronics. Here, we report a synergetic strategy to induce and modulate the ferromagnetism of the originally nonmagnetic MoS2 nanosheets. A two-step experimental method was used to simultaneously introduce substitutional V dopants and sulfur vacancy (Vs) in the MoS2 nanosheet host, showing an air-stable and adjustable ferromagnetic response at room temperature. The ferromagnetism could be modulated by varying the content of Vs through Ar plasma irradiation of different periods, with a maximum saturation magnetization of 0.011 emu g-1 reached at the irradiation time of 6 s (s). Experimental characterizations and first-principles calculations suggest that the adjustable magnetization is attributed to the synergetic effect of the substitutional V dopants and Vs in modulating the band structure of MoS2 nanosheets, resulting from the strong hybridization between the V 3d state and the Vs-induced impurity bands. This work suggests that the synergetic effect of substitutional V atoms and Vs is a promising route for tuning the magnetic interactions in two-dimensional nanostructures.
Keywords: magnetic MoS nanosheets; strong hybridization; substitutional dopants; sulfur vacancy; synergetic effect.