Van der Waals materials provide a versatile toolbox for the emergence of new quantum phenomena and the fabrication of functional heterostructures. Among them, the trihalide VI3 stands out for its unique magnetic and structural landscape. Here we investigate the spin and orbital magnetic degrees of freedom in the layered ferromagnet VI3 by means of temperature-dependent x-ray absorption spectroscopy and x-ray magnetic circular and linear dichroism. We detect localized electronic states and reduced magnetic dimensionality, due to electronic correlations. We furthermore provide experimental evidence of (a) an unquenched orbital magnetic moment (up to 0.66(7)) in the ferromagnetic state, and (b) an instability of the orbital moment in proximity of the spin reorientation transition. Our results support a coherent picture where electronic correlations give rise to a strong magnetic anisotropy and a large orbital moment, and establish VI3 as a prime candidate for the study of orbital quantum effects.
The recent emergence of two-dimensional (2D) van der Waals ferromagnets has provided a new platform for exploring magnetism in the flatland and for designing 2D ferromagnet-based spintronics devices. Despite intensive studies, the anomalous Hall effect (AHE) mechanisms in 2D van der Waals ferromagnets have not been investigated yet. In this paper, we report the AHE mechanisms in quasi-2D van der Waals ferromagnet Fe0.29TaS2 via systematically measuring Fe0.29TaS2 devices with thickness from 14 nm to bulk single crystal. The AHE mechanisms are investigated via the scaling relationship between t…
We examined what interactions control the sign and strength of the interlayer coupling in van der Waals ferromagnets such as Fe3-xGeTe2, Cr2Ge2Te6, CrI3 and VI3, to find that high-spin orbital interaction across the van der Waals gaps are a key to understanding their ferromagnetism. Interlayer ferromagnetic coupling in Fe3-xGeTe2 Cr2Ge2Te6, and CrI3 is governed by the high-spin two-orbital two-electron destabilization, but that in VI3 by the high-spin four-orbital two-electron stabilization. These interactions explain a number of seemingly puzzling observations in van der Waals fer-romagnets.
In order to investigate the electronic properties of the semiconducting van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$ (CGT), where ferromagnetic layers are bonded through van der Waals forces, we have performed angle-resolved photoemission spectroscopy (ARPES) measurements and density-functional-theory (DFT+U) calculations. The valence-band maximum at the Γ point is located $\sim$ 0.2 eV below the Fermi level, consistent with the semiconducting property of CGT. Comparison of the experimental density of states with the DFT calculation has suggested that Coulomb interaction between the Cr 3d elec…
Among the recently widely studied van der Waals layered magnets CrX3 (X=Cl, Br, I), CrCl3 monolayer (ML) is particularly puzzling as it is solely shown by experiments to have an in-plane magnetic easy axis and, furthermore, all of previous first-principles calculation results contradict this. Through systematical first-principles calculations,we unveil that its in-plane shape anisotropy that dominates over its weak perpendicular magnetocrystalline anisotropy is responsible for the in-plane magnetic easy axis of CrCl3 ML. To tune the in-plane ferromagnetism of CrCl3 ML into the desirable perpen…
We investigated the Dirac-cone state and its modulation when an ultrathin film of topological insulator Bi2Se3 was epitaxially grown on a van-der-Waals ferromagnet Cr2Si2Te6 (CST) by angle-resolved photoemission spectroscopy. We observed a gapless Dirac-cone surface state in 6 quintuple-layer (QL) Bi2Se3 on CST, whereas the Dirac cone exhibits a gap of 0.37 eV in 2QL counterpart. Intriguingly, this gap is much larger than those for Bi2Se3 films on Si(111). We also revealed no discernible change in the gap magnitude across the ferromagnetic transition of CST, suggesting the very small character…
Electronic structure of layered van der Waals ferromagnet CrI$_{3}$ is studied with self consistent diagrammatic approaches beyond GW approximation. Considerable improvement in the calculated band gap as compared to the non-self-consistent G0W0 results has been found. Certain spectral features in the valence bands discovered recently by the angle resolved photoemission spectroscopy, are reproduced better when we use full frequency dependent self energy. Density functional theory and quasiparticle self-consistent GW method which are based on frequency-independent self energy are unable to resol…
Laser-Induced Topological Toggle Switching at Room Temperature in the van der Waals Ferromagnet Fe3GaTe2
University College London（伦敦大学学院）；Korea Advanced Institute of Science and Technology (KAIST)（韩国科学技术院）；University of Exeter（埃克塞特大学）；The University of Edinburgh（爱丁堡大学）
Identifying intrinsic low-dimensional ferromagnets with high transition temperature and electrically tunable magnetism is crucial for the development of miniaturized spintronics and magnetoelectrics. Recently long-range 2D ferromagnetism was observed in van der Waals crystals CrI$_3$ and Cr$_2$Ge$_2$Te$_6$, however their Curie temperature is significantly lowered when reducing down to monolayer/few layers. Herein, using renormalized spin-wave theory and first-principles electronic structure theory, we present a theoretical study of electrically tunable 2D ferromagnetism in van der Waals layere…
The discoveries of intrinsic ferromagnetism in atomically-thin van der Waals crystals have opened up a new research field enabling fundamental studies on magnetism at two-dimensional (2D) limit as well as development of magnetic van der Waals heterostructures. To date, a variety of 2D ferromagnetism has been explored mainly by mechanically exfoliating 'originally ferromagnetic (FM)' van der Waals crystals, while bottom-up approach by thin film growth technique has demonstrated emergent 2D ferromagnetism in a variety of 'originally non-FM' van der Waals materials. Here we demonstrate that V5Se8…
We use the synergy of infrared, terahertz, and Raman spectroscopies with DFT calculations to shed light on the magnetic and lattice properties of VI3. The structural transition at TS1 = 79 K is accompanied by a large splitting of polar phonon modes. Below TS1, strong ferromagnetic fluctuations are observed. The variations of phonon frequencies at 55 K induced by magnetoelastic coupling enhanced by spin-orbit interaction indicate the proximity of long-range ferromagnetic order. Below TC = 50 K, two Raman modes simultaneously appear and show dramatic softening in the narrow interval around the t…
Manipulation of long-range order in two-dimensional (2D) van der Waals (vdW) magnetic materials (e.g., CrI$_3$, CrSiTe$_3$ etc.), exfoliated in few-atomic layer, can be achieved via application of electric field, mechanical-constraint, interface engineering, or even by chemical substitution/doping. Usually, active surface oxidation due to the exposure in the ambient condition and hydrolysis in the presence of water/moisture causes degradation in magnetic nanosheets which, in turn, affects the nanoelectronic/spintronic device performance. Counterintuitively, our current study reveals that expos…
Low temperature magnetization of CrI3, CrSiTe3 and CrGeTe3 single crystals were systematically studied. Based on the temperature dependence of extrapolated spontaneous magnetization from magnetic isotherms measured at different temperatures, the spin stiffness constant (D) and spin excitation gap ($Δ$) were extracted according to Bloch's law. For spin stiffness, D is estimated to be 27${\pm}$6 meV $Å^2$, 20${\pm}$3 meV $Å^2$ and 38${\pm}$7 meV $Å^2$ for CrI3, CrSiTe3 and CrGeTe3 respectively. Spin excitation gaps determined via Bloch's formulation have larger error bars yielding 0.59${\pm}$0.3…
The existence of long range magnetic order in low dimensional magnetic systems, such as the quasi-two-dimensional (2D) van der Waals (vdW) magnets, has attracted intensive studies of new physical phenomena. The vdW Fe$_N$GeTe$_2$ ($N$ = 3, 4, 5; FGT) family is exceptional owing to its vast tunability of magnetic properties. Particularly, a ferromagnetic ordering temperature ($T_{\text{C}}$) above room temperature at $N$ = 5 (F5GT) is observed. Here, our study shows that, by nickel (Ni) substitution of iron (Fe) in F5GT, a record high $T_{\text{C}}$ = 478(6) K is achieved. Importantly, pervasiv…
In recent years, two-dimensional van der Waals materials have emerged as an important platform for the observation of long-range ferromagnetic order in atomically thin layers. Although heterostructures of such materials can be conceived to harness and couple a wide range of magneto-optical and magneto-electrical properties, technologically relevant applications require Curie temperatures at or above room-temperature and the ability to grow films over large areas. Here we demonstrate the large-area growth of single-crystal ultrathin films of stoichiometric Fe5GeTe2 on an insulating substrate us…
Coexistence of ferromagnetism and ferroelectricity in the van der Waals multiferroic CuIn0.2V0.8P2S6
D crystal consortium, Materials Research Institute, Pennsylvania State University（宾夕法尼亚州立大学材料研究所）；Department of Physics, Pennsylvania State University（宾夕法尼亚州立大学物理系）；Department of Electrical and Computer Engineering and Quantum Technology Center, University of Maryland（马里兰大学电气与计算机工程系及量子技术中心）；Department of Chemistry, Michigan State University（密歇根州立大学化学系）；Department of Materials Science and Engineering, Pennsylvania State University（宾夕法尼亚州立大学材料科学与工程系）
The recent emergence of magnetic van der Waals materials allows for the investigation of current induced magnetization manipulation in two dimensional materials. Uniquely, Fe3GeTe2 has a crystalline structure that allows for the presence of bulk spin-orbit torques (SOTs), that we quantify in a Fe3GeTe2 flake. From the symmetry of the measured torques, we identify the current induced effective fields using harmonic analysis and find dominant bulk SOTs, which arise from the symmetry in the crystal structure. Our results show that Fe3GeTe2 uniquely can exhibit bulk SOTs in addition to the convent…
Recently, van der Waals (vdW) magnetic heterostructures have received increasing research attention in spintronics. However, the lack of room-temperature magnetic order of vdW material has largely impedes its development in practical spintronics devices. Inspired by the recently discovered vdW ferromagnet Fe3GaTe2, which has been shown to have magnetic order above room temperature and sizable perpendicular magnetic anisotropy, we investigate the basic electronic structure and magnetic properties of Fe3GaTe2 as well as tunneling magnetoresistance effect in magnetic tunnel junctions (MTJs) with …
Charge transfer plays a key role at the interfaces of heterostructures, which can affect electronic structures and ultimately the physical properties of the materials. However, charge transfer is difficult to manipulate externally once the interface formed. Here, we report electrically tunable charge transfer in Fe3GeTe2/Cr2Ge2Te6/Fe3GeTe2 all-magnetic van der Waals heterostructures, which can be exploited to selectively modify the magnetic properties of the top or bottom Fe3GeTe2 electrodes. The directional charge transfer from metallic Fe3GeTe2 to semiconducting Cr2Ge2Te6 remarkably modifies…
The recent experimental discovery of intrinsic ferromagnetism in single-layer CrI3 opens a new avenue to low-dimensional spintronics. However, the low Curie temperature Tc=45 K is still a large obstacle to its realistic device application. In this work, we demonstrate that the Tc and magnetic moment of CrX3(X=Br, I) can be enhanced simultaneously by coupling them to buckled two-dimensional Mene (M=Si, Ge) to form magnetic van der Waals (vdW) heterostructures. Our first-principles calculations reveal that n-doping of CrX3, induced by a significant spin-dependent interlayer charge transfer from …
Among several well-known transition metal-based compounds, the van der Waals (vdW) Fe3-xGeTe2 (FGT) magnet is a strong candidate for use in two-dimensional (2D) magnetic devices due to its strong perpendicular magnetic anisotropy, sizeable Curie temperature (TC ~ 154 K), and versatile magnetic character that is retained in the low-dimensional limit. While the TC remains far too low for practical applications, there has been a successful push toward improving it via external driving forces such as pressure, irradiation, and doping. Here we present experimental evidence of a novel room-temperatu…
The recent discovery of magnetic van der Waals materials has triggered a wealth of investigations in materials science, and now offers genuinely new prospects for both fundamental and applied research. Although the catalogue of van der Waals ferromagnets is rapidly expanding, most of them have a Curie temperature below 300 K, a notable disadvantage for potential applications. Combining element-selective x-ray magnetic imaging and magnetic force microscopy, we resolve at room temperature the magnetic domains and domains walls in micron-sized flakes of the CrTe$_2$ van der Waals ferromagnet. Flu…
The van der Waals ferromagnet Fe$_3$GeTe$_2$ has recently attracted extensive research attention due to its intertwined magnetic, electronic and topological properties. Here, using high-resolution angle-resolved photoemission spectroscopy, we systematically investigate the temperature evolution of the electronic structure of bulk Fe$_3$GeTe$_2$. We observe largely dispersive energy bands that are narrowed by a factor of 1.6 compared with ab-initio calculation. Upon heating towards the ferromagnetic transition near 225 K, we observe a massive reduction of quasiparticle coherence in a large ener…
The recent isolation of two-dimensional (2D) magnets offers tantalizing opportunities for spintronics and magnonics at the limit of miniaturization. One of the key advantages of atomically-thin materials is their outstanding deformation capacity, which provides an exciting avenue to control their properties by strain engineering. Herein, we investigate the magnetic properties, magnon dispersion and spin dynamics of the air-stable 2D magnetic semiconductor CrSBr ($T_C$ = 146 K) under mechanical strain using first-principles calculations. Our results provide a deep microscopic analysis of the co…
We have synthesized unique colloidal nanoplatelets of the ferromagnetic two-dimensional (2D) van der Waals material CrI3 and have characterized these nanoplatelets structurally, magnetically, and by magnetic circular dichroism spectroscopy. The isolated CrI3 nanoplatelets have lateral dimensions of ~25 nm and ensemble thicknesses of only ~4 nm, corresponding to just a few CrI3 monolayers. Magnetic and magneto-optical measurements demonstrate robust 2D ferromagnetic ordering in these nanoplatelets with Curie temperatures similar to those observed in bulk CrI3, despite the strong spatial confine…
Ferromagnetic semiconductors discovered in two-dimensional (2D) materials open an avenue for highly integrated and multifunctional spintronics. The Curie temperature (TC) of existed 2D ferromagnetic semiconductors is extremely low and the modulation effect of their magnetism is limited compared with their 2D metallic counterparts. The interfacial effect was found to effectively manipulate the three-dimensional magnetism, providing a unique opportunity for tailoring the 2D magnetism. Here we demonstrate that the TC of 2D ferromagnetic semiconductor Cr2Ge2Te6 can be enhanced by 130% (from ~65 K …
Controlling the magnetic anisotropy of ferromagnetic materials plays a key role in magnetic switching devices and spintronic applications. Examples of spin-orbit torque devices with different magnetic anisotropy geometries (in-plane or out-of-plane directions) have been demonstrated with novel magnetization switching mechanisms for extended device functionalities. Normally, the intrinsic magnetic anisotropy in ferromagnetic materials is unchanged within a fixed direction, and thus, it is difficult to realize multifunctionality devices. Therefore, continuous modulation of magnetic anisotropy in…
Ferromagnetism in two-dimensional materials presents a promising platform for the development of ultrathin spintronic devices with advanced functionalities. Recently discovered ferromagnetic van der Waals crystals such as CrI$_{3}$, readily isolated two-dimensional crystals, are highly tunable through external fields or structural modifications. However, there remains a challenge because of material instability under air exposure. Here, we report the observation of an air stable and layer dependent ferromagnetic (FM) van der Waals crystal, CrPS$_{4}$, using magneto-optic Kerr effect microscopy…
Low dimensional magnetism has been powerfully boosted as a promising candidate for numerous applications. The stability of the long-range magnetic order is directly dependent on the electronic structure and the relative strength of the competing magnetic exchange constants. Here, we report a comparative pressure-dependent theoretical and experimental study of the electronic structure and exchange interactions of two-dimensional ferromagnets CrBr3 and Cr2Ge2Te6 . While CrBr3 is found to be a Mott-Hubbard-like insulator, Cr2Ge2Te6 shows a charge-transfer character due to the broader character of…
We measure spin-orbit torque generated by exfoliated layers of the low-symmetry semi-metal ZrTe$_3$ using the spin-torque ferromagnetic resonance (ST-FMR) technique. When the ZrTe$_3$ has a thickness greater than about 10 nm, artifacts due to spin pumping and/or resonant heating can cause the standard ST-FMR analysis to overestimate the true magnitude of the torque efficiency by as much as a factor of 30, and to indicate incorrectly that the spin-orbit torque depends strongly on the ZrTe$_3$ layer thickness. Artifact-free measurements can still be achieved over a substantial thickness range by…
Since the discovery of ferromagnetic two-dimensional (2D) van der Waals (vdW) crystals, significant interest on such 2D magnets has emerged, inspired by their appealing properties and integration with other 2D family for unique heterostructures. In known 2D magnets, spin-orbit coupling (SOC) stabilizes perpendicular magnetic anisotropy (PMA). Such a strong SOC could also lift the chiral degeneracy, leading to the formation of topological magnetic textures such as skyrmions through the Dzyaloshinskii-Moriya interaction (DMI). Here, we report the experimental observation of Néel-type chiral magn…
Understanding the physics of phase transitions in two-dimensional (2D) systems underpins the research in diverse fields including statistical mechanics, quantum systems, nanomagnetism, and soft condensed matter. However, many fundamental aspects of 2D phase transitions are still not well understood, including the effects of interparticle potential, polydispersity, and particle shape. Magnetic skyrmions, which are non-trivial chiral spin structures, can be considered as quasi-particles that form two-dimensional lattices. Here we show, by real-space imaging using in situ cryo-Lorentz transmissio…
In this work, we reported the observation of a novel planar topological Hall effect (PTHE) in single crystal of Fe3GeTe2, a paradigmatic two-dimensional ferromagnet with strong uniaxial anisotropy. The Hall effect and magnetoresistance varied periodically when the external magnetic field rotated in the ac (or bc) plane, while the PTHE emerged and maintained robust with field swept across the hard-magnetized ab plane. The PTHE covers the whole temperature region below Tc (~150 K) and a comparatively large value is observed at 100 K. Emergence of an internal gauge field was proposed to explain t…
Intrinsic ferromagnetism is a crucial ingredient to realize quantum anomalous Hall effect in quasi two dimensional materials, thus the search of intrinsic ferromagnetic topological materials is one of the most concerned issues in the field of topological phases of matter. In this work, combining magnetotransport measurements, first principles calculations, and angle-resolved photoemission spectroscopy studies, we find that in MnSb6Te10, the n = 2 member of the MnSb2Te4/(Sb2Te3)n family, the strong magnetic competition realizes a fragile ferromagnetic ground state, which whereas easily enters i…
Strain-Mediated Lattice Reconstruction Enhances Ferromagnetism in Cr2Ge2Te6/WTe2 van der Waals Heterobilayers
Catalan Institute of Nanoscience and Nanotechnology (ICN2), CSIC and the Barcelona Institute of Science and Technology (BIST)（加泰罗尼亚纳米科学和纳米技术研究所（ICN2），西班牙高等科学研究委员会（CSIC）和巴塞罗那科学与技术研究所（BIST））；Universitat Autònoma de Barcelona（巴塞罗那自治大学）；Institut de Ciència de Materials de Barcelona, ICMAB-CSIC（巴塞罗那材料科学研究所，西班牙高等科学研究委员会（ICMAB-CSIC））；Research Center for Electronic and Optical Materials, National Institute for Materials Science（电子与光学材料研究中心，日本物质材料研究机构）；Research Center for Materials Nanoarchitectonics, National Institute for Materials Science（材料纳米结构研究中心，日本物质材料研究机构）；Institute of Optical Materials and Technologies, Bulgarian Academy of Science（保加利亚科学院光学材料与技术研究所）；Institute of Solid State Physics, Bulgarian Academy of Sciences（保加利亚科学院固体物理研究所）；Quantum Innovation Centre (Q. InC), Agency for Science Technology and Research (A*STAR)（量子创新中心（Q. InC），新加坡科技研究局（A*STAR））
A comprehensive study of magnetocrystalline anisotropy of a layered van-der-Waals ferromagnet VI3 was performed. We measured angular dependences of the torque and magnetization with respect to the direction of the applied magnetic field within the "ac" plane perpendicular to and within the basal ab plane, respectively. A two-fold butterfly-like signal was detected by magnetization in the perpendicular "ac" plane. This signal symmetry remains conserved throughout all magnetic regimes as well as through the known structural transition down to the lowest temperatures. The maximum of the magnetiza…
Broadening the knowledge and understanding on the magnetic correlations in van der Waals layered magnets is critical in realizing their potential next-generation applications. In this study, we employ high frequency (240 GHz) electron spin resonance (ESR) spectroscopy on plate-like CrBr$_{3}$ to gain insight into the magnetic interactions as a function of temperature (200 - 4 K) and the angle of rotation $θ$. We find that the temperature dependence of the ESR linewidth is well described by the Ginzberg-Landau critical model as well as Berezinskii-Kosterlitz-Thouless (BKT) transition model, ind…
Magnomechanical Coupling in Suspended 2D van der Waals Ferromagnets
Kavli Institute of Nanoscience, Delft University of Technology（代尔夫特理工大学卡弗里纳米科学研究所）；Department of Precision and Microsystems Engineering, Delft University of Technology（代尔夫特理工大学精密与微系统工程系）
Spontaneous Enhancement of Dzyaloshinskii-Moriya Interaction via Field-Cooling-Induced Interface Engineering in 2D van der Waals Ferromagnetic ternary Tellurides
Wuhan University（武汉大学）；Southeast University（东南大学）；Yanshan University（燕山大学）；Beihang University（北京航空航天大学）；Wuhan Institute of Quantum Technology（武汉量子技术研究院）
We demonstrate that kinetics play an important role in the epitaxial growth of Fe$_3$GeTe$_2$ (FGT) van der Waals (vdW) ferromagnetic films by molecular beam epitaxy. By varying the deposition rate, we control the formation or suppression of an initial tellurium-deficient non-van der Waals phase (Fe$_3$Ge$_2$) prior to realizing epitaxial growth of the vdW FGT phase. Using cross-sectional scanning transmission electron microscopy and scanning tunneling microscopy, we optimize the FGT films to have atomically smooth surfaces and abrupt interfaces with the Ge(111) substrate. The magnetic propert…
Emergent color centers with accessible spins hosted by van der Waals materials have attracted substantial interest in recent years due to their significant potential for implementing transformative quantum sensing technologies. Hexagonal boron nitride (hBN) is naturally relevant in this context due to its remarkable ease of integration into devices consisting of low-dimensional materials. Taking advantage of boron vacancy spin defects in hBN, we report nanoscale quantum imaging of low-dimensional ferromagnetism sustained in Fe3GeTe2/hBN van der Waals heterostructures. Exploiting spin relaxomet…
The intersection of topology and magnetism represents a new playground to discover novel quantum phenomena and device concepts. In this work, we show that a van der Waals compound MnSb$_{1.8}$Bi$_{0.2}$Te$_4$ exhibits a ferromagnetic ground state with a Curie temperature of 26 K, in contrast to the antiferromagnetic order previously found for other members of the Mn(Sb, Bi)$_2$Te$_4$ family. We employ magneto-transport, bulk magnetization and neutron scattering studies to illustrate the magnetic and electrical properties of MnSb$_{1.8}$Bi$_{0.2}$Te$_4$ and report on the observation of an unusu…
