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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 CrxGa1−xTe crystals exhibiting highly tunable above‐room‐temperature ferromagnetism with bandgap 1.62–1.66 eV are reported. The saturation magnetic moment (Msat) of CrxGa1−xTe crystals can be effectively regulated up to ≈5.4 times by tuning Cr content and ≈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 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. [ABSTRACT FROM AUTHOR]

Abstract: The Weyl semimetal WTe2 and MoTe2 show great potential in generating large spin currents since they possess topologically protected spin‐polarized states and can carry a very large current density. In addition, the intrinsic non‐centrosymmetry of WTe2 and MoTe2 endows with a unique property of crystal symmetry‐controlled spin–orbit torques. An important question to be answered for developing spintronic devices is how spins relax in WTe2 and MoTe2. Here, a room‐temperature spin relaxation time of 1.2 ns (0.4 ns) in WTe2 (MoTe2) thin film using the time‐resolved Kerr rotation (TRKR) is reported. Based on ab initio calculation, a mechanism of long‐lived spin polarization resulting from a large spin splitting around the bottom of the conduction band, low electron–hole recombination rate, and suppression of backscattering required by time‐reversal and lattice symmetry operation is identified. In addition, it is found that the spin polarization is firmly pinned along the strong internal out‐of‐plane magnetic field induced by large spin splitting. This work provides an insight into the physical origin of long‐lived spin polarization in Weyl semimetals, which could be useful to manipulate spins for a long time at room temperature. [ABSTRACT FROM AUTHOR]