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One primary concern in diluted magnetic semiconductors (DMSs) is how toestablish a long-range magnetic order with a low magnetic doping concentrationto maintain the gate tunability of the host semiconductor, as well as toincrease Curie temperature. Two-dimensional van der Waals semiconductors havebeen recently investigated to demonstrate the magnetic order in DMSs; however,a comprehensive understanding of the mechanism responsible for the gate-tunablelong-range magnetic order in DMSs has not been achieved yet. Here, we introducea monolayer tungsten diselenide (WSe2) semiconductor with V dopants todemonstrate the long-range magnetic order through itinerant spin-polarizedholes. The V atoms are sparsely located in the host lattice by substituting Watoms, which is confirmed by scanning tunneling microscopy and high-resolutiontransmission electron microscopy. The V impurity states and the valence bandedge states are overlapped, which is congruent with density functional theorycalculations. The field-effect transistor characteristics reveal the itinerantholes within the hybridized band; this clearly resembles the Zener model. Ourstudy gives an insight into the mechanism of the long-range magnetic order inV-doped WSe2, which can also be used for other magnetically dopedsemiconducting transition metal dichalcogenides.

Evidence of itinerant holes for long-range magnetic order in tungsten diselenide semiconductor with vanadium dopants