Magnetic Transition in Monolayer VSe₂ <i>via</i> Interface Hybridization

Magnetism in monolayer (ML) VSe₂ has attracted broad interest in spintronics, while existing reports have not reached consensus. Using element-specific X-ray magnetic circular dichroism, a magnetic transition in ML VSe₂ has been demonstrated at the contamination-free interface between Co and VSe₂. Through interfacial hybridization with a Co atomic overlayer, a magnetic moment of about 0.4 μ_B per V atom in ML VSe₂ is revealed, approaching values predicted by previous theoretical calculations. Promotion of the ferromagnetism in ML VSe₂ is accompanied by its antiferromagnetic coupling to Co and a reduction in the spin moment of Co. In comparison to the absence of this interface-induced ferromagnetism at the Fe/ML MoSe₂ interface, these findings at the Co/ML VSe₂ interface provide clear proof that the ML VSe₂, initially with magnetic disorder, is on the verge of magnetic transition.