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Magnetism in monolayer (ML) VSe2 has attracted broad interest in spintronicswhile existing reports have not reached consensus. Using element-specific X-raymagnetic circular dichroism, a magnetic transition in ML VSe2 has beendemonstrated at the contamination-free interface between Co and VSe2. Viainterfacial hybridization with Co atomic overlayer, a magnetic moment of about0.4 uB per V atom in ML VSe2 is revealed, approaching values predicted byprevious theoretical calculations. Promotion of the ferromagnetism in ML VSe2is accompanied by its antiferromagnetic coupling to Co and a reduction in thespin moment of Co. In comparison to the absence of this interface-inducedferromagnetism at the Fe/MLMoSe2 interface, these findings at the Co/ML-VSe2interface provide clear proof that the ML VSe2, initially with magneticdisorder, is on the verge of magnetic transition.

Magnetic Transition in Monolayer VSe2 via Interface Hybridization