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 (TC ) 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 Crx Ga1-x Te crystals exhibiting highly tunable above-room-temperature ferromagnetism with bandgap 1.62-1.66 eV are reported. The saturation magnetic moment (Msat ) of Crx Ga1-x Te crystals can be effectively regulated up to ≈5.4 times by tuning Cr content and ≈75.9 times by changing the thickness. vdW Crx Ga1-x Te ultrathin semiconductor crystals show robust room-temperature ferromagnetism with the 2D quantum confinement effect, enabling TC 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.