While the discovery of two-dimensional (2D) magnets opens the door for fundamental physics and next-generation spintronics, it is technically challenging to achieve the room-temperature ferromagnetic (FM) order in a way compatible with potential device applications. Here, we report the growth and properties of single- and few-layer CrTe2, a van der Waals (vdW) material, on bilayer graphene by molecular beam epitaxy (MBE). Intrinsic ferromagnetism with a Curie temperature (TC) up to 300 K, an atomic magnetic moment of ~0.21 $${\mu }_{{\rm{B}}}$$ μ B /Cr and perpendicular magnetic anisotropy (PMA) constant (Ku) of 4.89 × 105 erg/cm3 at room temperature in these few-monolayer films have been unambiguously evidenced by superconducting quantum interference device and X-ray magnetic circular dichroism. This intrinsic ferromagnetism has also been identified by the splitting of majority and minority band dispersions with ~0.2 eV at Г point using angle-resolved photoemission spectroscopy. The FM order is preserved with the film thickness down to a monolayer (TC ~ 200 K), benefiting from the strong PMA and weak interlayer coupling. The successful MBE growth of 2D FM CrTe2 films with room-temperature ferromagnetism opens a new avenue for developing large-scale 2D magnet-based spintronics devices.

Mechanically exfoliated two-dimensional ferromagnetic materials (2D FMs) possess long-range ferromagnetic order and topologically nontrivial skyrmions in few layers. However, because of the dimensionality effect, such few-layer systems usually exhibit much lower Curie temperature (TC) compared to their bulk counterparts. It is therefore of great interest to explore effective approaches to enhance their TC, particularly in wafer-scale for practical applications. Here, we report an interfacial proximity-induced high-TC 2D FM Fe3GeTe2 (FGT) via A-type antiferromagnetic material CrSb (CS) which strongly couples to FGT. A superlattice structure of (FGT/CS)n, where n stands for the period of FGT/CS heterostructure, has been successfully produced with sharp interfaces by molecular-beam epitaxy on 2-inch wafers. By performing elemental specific X-ray magnetic circular dichroism (XMCD) measurements, we have unequivocally discovered that TC of 4-layer Fe3GeTe2 can be significantly enhanced from 140 K to 230 K because of the interfacial ferromagnetic coupling. Meanwhile, an inverse proximity effect occurs in the FGT/CS interface, driving the interfacial antiferromagnetic CrSb into a ferrimagnetic state as evidenced by double-switching behavior in hysteresis loops and the XMCD spectra. Density functional theory calculations show that the Fe-Te/Cr-Sb interface is strongly FM coupled and doping of the spin-polarized electrons by the interfacial Cr layer gives rise to the TC enhancement of the Fe3GeTe2 films, in accordance with our XMCD measurements. Strikingly, by introducing rich Fe in a 4-layer FGT/CS superlattice, TC can be further enhanced to near room temperature. Our results provide a feasible approach for enhancing the magnetic order of few-layer 2D FMs in wafer-scale and render opportunities for realizing realistic ultra-thin spintronic devices.

As an emerging class of two-dimensional (2D) materials, van der Waals (vdW) magnets have attracted a lot of research attention since they can give access to fundamental physics and potential spintronic device applications. Among these 2D vdW magnets, CrSiTe3, as an intrinsic ferromagnetic semiconductor, exhibits great potentials in low-dimensional spintronics. Of particular interest in this 2D vdW magnet is the electronic and magnetic properties at the atomic-scale, which has yet been fully explored so far. Here, combing angle-resolved photoemission spectroscopy, bulk magnetic measurements, and synchrotron-based x-ray techniques, an unambiguous picture of the electronic and magnetic states of CrSiTe3 is presented. Hybridization of Cr-3d and Te-5p orbitals and the semiconducting behavior are confirmed by the band structure detection. Intrinsic ferromagnetism with a magnetic anisotropy constant of 1.56 × 105 erg/cm3 is attributed to the superexchange interaction of the Cr3+ ions. In addition, temperature-dependent spin and orbital moments are determined, and a fitted critical exponent of 0.169 implies that CrSiTe3 is in good agreement with the 2D Ising model. More remarkably, unquenched orbital moments are experimentally evidenced, bringing CrSiTe3 with orbital-dependent intriguing effects and great potentials toward the spintronic devices.

One of the most promising avenues in 2D materials research is the synthesis of antiferromagnets employing 2D van der Waals (vdW) magnets. However, it has proven challenging, due in part to the complicated fabrication process and undesired adsorbates as well as the significantly deteriorated ferromagnetism at atomic layers. Here, the engineering of the antiferromagnetic (AFM) interlayer exchange coupling between atomically thin yet ferromagnetic CrTe 2 layers in an ultra-high vacuum-free 2D magnetic crystal, Cr 5 Te 8 is reported. By self-introducing interstitial Cr atoms in the vdW gaps, the emergent AFM ordering and the resultant giant magnetoresistance effect are induced. A large negative magnetoresistance (10%) with a plateau-like feature is revealed, which is consistent with the AFM interlayer coupling between the adjacent CrTe 2 main layers in a temperature window of 30 K below the Néel temperature. Notably, the AFM state has a relatively weak interlayer exchange coupling, allowing a switching between the interlayer AFM and ferromagnetic states at moderate magnetic fields. This work represents a new route to engineering low-power devices that underpin the emerging spintronic technologies, and an ideal laboratory to study 2D magnetism.

Two-dimensional (2D) ferromagnetic materials have been discovered with tunable magnetism and orbital-driven nodal-line features. Controlling the 2D magnetism in exfoliated nanoflakes via electric/magnetic fields enables the boosted Curie temperature (TC) or phase transitions. One of the challenges, however, is the realization of high TC 2D magnets that are tunable, robust and suitable for large scale fabrication. Here, we report molecular-beam epitaxy growth of wafer-scale Fe3+XGeTe2 films with TC above-room-temperature. By controlling the Fe composition in Fe3+XGeTe2, a continuously-modulated TC in a broad range of 185–320 K has been achieved. This widely tunable TC is attributed to the doped interlayer Fe that provide a 40% enhancement around the optimal composition X = 2. We further fabricated magnetic tunneling junction device arrays that exhibit clear tunneling signals. Our results show an effective and reliable approach, i.e. element doping, to produce robust and tunable ferromagnetism beyond room temperature in a large-scale 2D Fe3+XGeTe2 fashion.