Highly‐Tunable Intrinsic Room‐Temperature Ferromagnetism in 2D van der Waals Semiconductor Cr_xGa_1−xTe

Abstract 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 Cr_xGa_1−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 Cr_xGa_1−xTe crystals can be effectively regulated up to ≈5.4 times by tuning Cr content and ≈75.9 times by changing the thickness. vdW Cr_xGa_1−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.