Cr2Ge2Te6 is a van der Waals ferromagnet with a Curie temperature at 66 K. Here we report a swift change in the magnetic ground state upon application of small DC electric current, a giant yet anisotropic magnetoelectric effect, and a sharp, lattice-driven quantum switching manifested in the I-V characteristic of the bulk single-crystal Cr2Ge2Te6. At the heart of these observed phenomena is a newly uncovered, strongly anisotropic magnetoelastic coupling that enables strongly anisotropic responses of the lattice to application of electric current and/or magnetic field, thus the exotic phenomena in Cr2Ge2Te6. Such a rare mechanical tunability in the magnetic semiconductors promises tantalizing prospects for unique functional materials and devices.
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.
We report an experimental discovery of CrSnS3, a new Van der Waals ferromagnetic (FM) with Curie temperature TC ~119K. The Curie temperature is in qualitative agreement of Chittari et. al. DFT prediction (TC =112.3K) for an Ising model with the addition of Coulomb potential. The FM ordering temperature in CrSnS3 is the highest among Cr-based Van der Waals materials: CrI3, CrSiTe3 and CrGeTe3. The dc-susceptibility revealed a sharp increase at Tc (~119K) indicative of a first order transition; then raises to a wide maximum at AFM Neel temperature TN~90K.The ac-susceptibility reveals the presenc…
Fe3-xGeTe2 is a layered magnetic van der Waals material of interest for both fundamental and applied research. Despite the observation of intriguing physical properties, open questions exist even on the basic features related to magnetism: is it a simple ferromagnet or are there antiferromagnetic regimes and are the moments local or itinerant. Here, we demonstrate that antiferromagnetic spin fluctuations coexist with the ferromagnetism through comprehensive elastic and inelastic neutron scattering and thermodynamic measurements. Our realistic dynamical mean-field theory calculations reveal tha…
We report structural, physical properties and electronic structure of van der Waals (vdW) crystal VI3. Detailed analysis reveals that VI3 exhibits a structural transition from monoclinic C2/m to rhombohedral R-3 at Ts ~ 79 K, similar to CrX3 (X = Cl, Br, I). Below Ts, a long-range ferromagnetic (FM) transition emerges at Tc ~ 50 K. The local moment of V in VI3 is close to the high-spin state V3+ ion (S = 1). Theoretical calculation suggests that VI3 may be a Mott insulator with the band gap of about 0.84 eV. In addition, VI3 has a relative small interlayer binding energy and can be exfoliated …
Van der Waals magnet VI$_3$ demonstrates intriguing magnetic properties that render it great for use in various applications. However, its microscopic magnetic structure has not been determined yet. Here, we report neutron diffraction and susceptibility measurements in VI$_3$ that revealed a ferromagnetic order with the moment direction tilted from the $c$-axis by ~36° at 4 K. A spin reorientation accompanied by a structure distortion within the honeycomb plane is observed at a temperature of ~27 K, before the magnetic order completely disappears at $T_C$ = 50 K. The refined magnetic moment of…
A complex interplay of different energy scales involving Coulomb repulsion, spin-orbit coupling and Hund's coupling energy in two-dimensional (2D) van der Waals (vdW) material produces novel emerging physical state. For instance, ferromagnetism in vdW charge transfer insulator CrGeTe$_3$, that provides a promising platform to simultaneously manipulate the magnetic and electrical properties for potential device implementation using few layers thick materials. Here, we show a continuous tuning of magnetic and electrical properties of CrGeTe$_3$ single crystal using pressure. With application of …
The bosonic analogues of topological insulators have been proposed in numerous theoretical works, but their experimental realization is still very rare, especially for spin systems. Recently, two-dimensional (2D) honeycomb van der Waals (vdW) ferromagnets have emerged as a new platform for topological spin excitations. Here, via a comprehensive inelastic neutron scattering study and theoretical analysis of the spin-wave excitations, we report the realization of topological magnon insulators in CrXTe$_3$ (X=Si, Ge) compounds. The nontrivial nature and intrinsic tunability of the gap opening at …
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 report a comprehensive high-field/high-frequency electron spin resonance (ESR) study on single crystals of the van der Waals magnet CrCl$_3$. This material, although being known for quite a while, has received recent significant attention in a context of the use of van der Waals magnets in novel spintronic devices. Temperature-dependent measurements of the resonance fields were performed between 4 and 175 K and with the external magnetic field applied parallel and perpendicular to the honeycomb planes of the crystal structure. These investigations reveal that the resonance line shifts from …
The magnetic structure and phase diagram of the layered ferromagnetic compound Fe$_3$GeTe$_2$ has been investigated by a combination of synthesis, x-ray and neutron diffraction, high resolution microscopy, and magnetization measurements. Single crystals were synthesized by self-flux reactions, and single crystal neutron diffraction finds ferromagnetic order with moments of 1.11(5)$μ_B$/Fe aligned along the $c$-axis at 4K. These flux-grown crystals have a lower Curie temperature $T_{\textrm{c}}\approx$150K compared to crystals previously grown by vapor transport ($T_{\textrm{c}}$=220K). The dif…
Van-der-Waals (vdW) ferromagnets have enabled the development of heterostructures assembled from exfoliated monolayers with spintronics functionalities, making it important to understand and ultimately tune their magnetic properties at the microscopic level. Information about the magnetic properties of these systems comes so far largely from macroscopic techniques, with little being known about the microscopic magnetic properties. Here, we combine spin-polarized scanning tunneling microscopy and quasi-particle interference imaging with neutron scattering to establish the magnetic and electroni…
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 weak antilocalization (WAL) effect is known as a quantum correction to the classical conductivity, which never appeared in two-dimensional magnets. In this work, we reported the observation of a WAL effect in the van der Waals ferromagnet Fe5-xGeTe2 with a Curie temperature Tc ~ 270 K, which can even reach as high as ~ 120 K. The WAL effect could be well described by the Hikami-Larkin-Nagaoka and Maekawa-Fukuyama theories in the presence of strong spin-orbit coupling (SOC). Moreover, A crossover from a peak to dip behavior around 60 K in both the magnetoresistance and magnetoconductance wa…
Two-dimensional (2D) van der Waals (vdW) magnets have been a fertile playground for the discovery and exploration of physical phenomena and new physics. In this Letter, we report the observation of an anomalous thermal Hall effect (THE) with \k{appa}_xy ~ 1x10^(-2) W K^(-1) m^(-1) in an insulating van der Waals ferromagnet VI3. The thermal Hall signal persists in the absence of an external magnetic field and flips sign upon the switching of the magnetization. In combination with theoretical calculations, we show that VI3 exhibits a dual nature of the THE, i.e., dominated by topological magnons…
We present comprehensive measurements of the structural, magnetic and electronic properties of layered van-der-Waals ferromagnet VI$_3$ down to low temperatures. Despite belonging to a well studied family of transition metal trihalides, this material has received very little attention. We outline, from high-resolution powder x-ray diffraction measurements, a corrected room-temperature crystal structure to that previously proposed and uncover a structural transition at 79 K, also seen in the heat capacity. Magnetization measurements confirm VI$_3$ to be a hard ferromagnet (9.1 kOe coercive fiel…
Orbital mixing and strong Hund's coupling stabilize spin order in van der Waals ferromagnet CrI3
Technische Universität Berlin（柏林工业大学）；Fritz Haber Institute of the Max Planck Society（马克斯·普朗克学会弗里茨·哈伯研究所）；Vinča Institute of Nuclear Sciences - National Institute of the Republic of Serbia, University of Belgrade（贝尔格莱德大学文查核科学研究所）；ESRF, The European Synchrotron（欧洲同步辐射装置）；Politecnico di Milano（米兰理工大学）；Consiglio Nazionale delle Ricerche CNR-IOM, Unità di Trieste（国家研究委员会CNR-IOM的里雅斯特分部）；University of Milan-Bicocca（米兰比可卡大学）；Consiglio Nazionale delle Ricerche CNR-SPIN, c/o Università degli Studi ‘G. D’Annunzio’（国家研究委员会CNR-SPIN，挂靠阿布鲁佐大学）
Two-dimensional (2D) van der Waals (vdW) magnetic materials have garnered considerable attention owing to the existence of magnetic order down to atomic dimensions and flexibility towards interface engineering, offering an attractive platform to explore novel spintronic phenomena and functionalities. Understanding of the magnetoresistive properties and their correlation to the underlying magnetic configurations is essential for 2D vdW-based spintronic or quantum information devices. Among the promising candidates, vdW ferromagnet (FM) Fe3GeTe2 shows an unusual magnetotransport behavior, tunabl…
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 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…
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）
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…
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…
We investigate near-Fermi-energy (EF) element-specific electronic and spin states of ferromagnetic van der Waals (vdW) metal Fe5GeTe2. The soft x-ray angle-resolved photoemission spectroscopy (SX-ARPES) measurement provides spectroscopic evidence of localized Fe 3d band. We also find prominent hybridization between the localized Fe 3d band and the delocalized Ge/Te p bands. This picture is strongly supported from direct observation of the remarkable spin polarization of the ligand p bands near EF, using x-ray magnetic circular dichroism (XMCD) measurements. The strength of XMCD signal from lig…
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）
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}$0.3…
Magnetic anisotropy in the near-stoichiometric van der Waals ferromagnet Fe$_3$GeTe$_2$
Leibniz Institute for Solid State and Materials Research（莱布尼茨固体与材料研究所）；Institute for Solid State and Materials Physics, TU Dresden（德累斯顿工业大学固体与材料物理研究所）；Department of Condensed Matter and Materials Physics, S. N. Bose National Centre for Basic Sciences（S.N. 玻色基础科学国家中心凝聚态与材料物理系）；School of Physical Sciences, Indian Association for the Cultivation of Science（印度科学促进协会物理科学学院）
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）
Quantum spin-liquid van der Waals magnets such as TaS$_2$, TaSe$_2$, and RuCl$_3$ provide a natural platform to explore new exotic phenomena associated with spinon physics, whose properties can be controlled by exchange proximity with ferromagnetic insulators such as CrBr$_3$. Here we put forward a twisted van der Waals heterostructure based on a quantum spin-liquid bilayer encapsulated between ferromagnetic insulators. We demonstrate the emergence of spinon flat bands and topological spinon states in such heterostructure, where the emergence of a topological gap is driven by the twist. We fur…
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 …
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…
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 …
