Highly-Tunable Intrinsic Room-Temperature Ferromagnetism in 2D van der Waals Semiconductor CrxGa1-xTe

The combination of semiconductivity and tunable ferromagnetism is pivotal for electrical control of ferromagnetism and next-generation low-power spintronic devices. However, Curie temperatures (T-C) for most traditional intrinsic ferromagnetic semiconductors (<= 200 K) and recently discovered two-dimensional (2D) ones (<70 K) are far below room temperature. 2D van der Waals (vdW) semiconductors with intrinsic room-temperature ferromagnetism remain elusive considering the unfavored 2D long-range ferromagnetic order indicated by Mermin-Wagner theorem. Here, vdW semiconductor CrxGa1-xTe crystals exhibiting highly tunable above-room-temperature ferromagnetism with bandgap 1.62-1.66 eV are reported. The saturation magnetic moment (M-sat) of CrxGa1-xTe crystals can be effectively regulated up to approximate to 5.4 times by tuning Cr content and approximate to 75.9 times by changing the thickness. vdW CrxGa1-xTe ultrathin semiconductor crystals show robust room-temperature ferromagnetism with the 2D quantum confinement effect, enabling T-C 314.9-329 K for nanosheets, record-high for intrinsic vdW 2D ferromagnetic semiconductors. This work opens an avenue to room-temperature 2D vdW ferromagnetic semiconductor for 2D electronic and spintronic devices.