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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]

The discovery of type‐II Weyl semimetal states in layered transition metal dichalcogenides Td‐WTe2 indicates great potential for novel electronic, spintronic, and quantum devices. Theoretically, the interaction between the topological states and the magnetic ordered states of Td‐WTe2 enables the modulation of Weyl semimetal states by an external magnetic field. However, currently, ferromagnetism in layered Td‐WTe2 is still elusive and rarely observed. In this research, ferromagnetic order into WTe2 using magnetic chromium (Cr) doping with a two‐step Te flux strategy is introduced. The Curie temperature (Tc) and the ferromagnetic moment are well tuned with a Cr doping concentration. The Tc of the Cr‐doped layered Td‐WTe2 could be regulated from 182 to 283 K, which is close to room temperature. The saturation magnetic moment could be changed from 2.26 to 4.20 emu g–1, which is stronger than most values reported for these materials. Most intriguingly, the Cr‐doped layered Td‐WTe2 single crystals still exhibit semimetallic behavior and they possess very large magnetoresistance with obvious Shubnikov de Haas (SdH) quantum oscillations and an anomalous Hall effect. The findings offer feasible ways to induce and tune ferromagnetic orders in layered Td‐WTe2 and thus to control its topological phase with external magnetic fields. [ABSTRACT FROM AUTHOR]

Magnetic tunnel junctions (MTJs) are widely applied in spintronic devices for efficient spin detection through the imbalance of spin polarization at the Fermi level. The van der Waals (vdW) property of 2D magnets with atomically flat surfaces and negligible surface roughness greatly facilitates the development of MTJs, primarily in ferromagnets. Here, A‐type antiferromagnetism in 2D vdW single‐crystal (Fe0.8Co0.2)3GaTe2 is reported with TN ≈ 203 K in bulk and ≈ 185 K in 9‐nm nanosheets. The metallic nature and out‐of‐plane magnetic anisotropy make it a suitable candidate for MTJ electrodes. By constructing heterostructures based on (Fe0.8Co0.2)3GaTe2/WSe2/Fe3GaTe2, a large tunneling magnetoresistance (TMR) ratio of 180% at low temperature is obtained, with the TMR signal persisting at near‐room temperature 280 K. Furthermore, the TMR is tunable by the electric field, and the MTJ device operates stably with a low applied bias down to 1 mV (≈0.6 nA), highlighting its potential for energy‐efficient spintronic devices. This work opens up new opportunities for 2D antiferromagnetic spintronics and quantum devices. [ABSTRACT FROM AUTHOR]

Developing novel high‐temperature van der Waals ferromagnetic semiconductor materials and investigating their interface coupling effects with 2D topological semimetals are pivotal for advancing next‐generation spintronic and quantum devices. However, most van der Waals ferromagnetic semiconductors exhibit ferromagnetism only at low temperatures, limiting the proximity research on their interfaces with topological semimetals. Here, an intrinsic, van der Waals layered room‐temperature ferromagnetic semiconductor crystal, FeCr0.5Ga1.5Se4 (FCGS), is reported with a Curie temperature (TC) as high as 370 K, setting a new record for van der Waals ferromagnetic semiconductors. The saturation magnetization at low temperature (2 K) and room temperature (300 K) reaches 8.2 and 2.7 emu g−1, respectively. Furthermore, FCGS possesses a bandgap of ≈1.2 eV, which is comparable to the widely used commercial silicon. The FCGS/graphene 2D heterostructure exhibits an impeccably smooth and gapless interface, thereby inducing a robust van der Waals magnetic proximity coupling effect between FCGS and graphene. After the proximity coupling, graphene undergoes a charge carrier transition from electrons to holes, accompanied by a transition from non‐magnetic to ferromagnetic transport behavior with robust anomalous Hall effect (AHE). Notably, the van der Waals magnetic proximity‐induced AHE remains robust even up to 400 K. [ABSTRACT FROM AUTHOR]

The discovery of type‐II Weyl semimetal states in layered transition metal dichalcogenides Td‐WTe2 indicates great potential for novel electronic, spintronic, and quantum devices. Theoretically, the interaction between the topological states and the magnetic ordered states of Td‐WTe2 enables the modulation of Weyl semimetal states by an external magnetic field. However, currently, ferromagnetism in layered Td‐WTe2 is still elusive and rarely observed. In this research, ferromagnetic order into WTe2 using magnetic chromium (Cr) doping with a two‐step Te flux strategy is introduced. The Curie temperature (Tc) and the ferromagnetic moment are well tuned with a Cr doping concentration. The Tc of the Cr‐doped layered Td‐WTe2 could be regulated from 182 to 283 K, which is close to room temperature. The saturation magnetic moment could be changed from 2.26 to 4.20 emu g–1, which is stronger than most values reported for these materials. Most intriguingly, the Cr‐doped layered Td‐WTe2 single crystals still exhibit semimetallic behavior and they possess very large magnetoresistance with obvious Shubnikov de Haas (SdH) quantum oscillations and an anomalous Hall effect. The findings offer feasible ways to induce and tune ferromagnetic orders in layered Td‐WTe2 and thus to control its topological phase with external magnetic fields. [ABSTRACT FROM AUTHOR]