Pressure control of the magnetic anisotropy of the quasi-two-dimensional van der Waals ferromagnet Cr$_2$Ge$_2$Te$_6$
T. Sakurai, B. Rubrecht, L. T. Corredor, R. Takehara, M. Yasutani, J. Zeisner, A. Alfonsov, S. Selter, S. Aswartham, A. U. B. Wolter, B. Büchner, H. Ohta, V. Kataev
We report the results of the pressure-dependent measurements of the static magnetization and of the ferromagnetic resonance (FMR) of Cr$_2$Ge$_2$Te$_6$ to address the properties of the ferromagnetic phase of this quasi-two-dimensional van der Waals magnet. The static magnetic data at hydrostatic pressures up to 3.4 GPa reveal a gradual suppression of ferromagnetism in terms of a reduction of the critical transition temperature, a broadening of the transition width and an increase of the field necessary to fully saturate the magnetization $M_{\rm s}$. The value of $M_{\rm s} \simeq 3μ_{\rm B}$/Cr remains constant within the error bars up to a pressure of 2.8 GPa. The anisotropy of the FMR signal continuously diminishes in the studied hydrostatic pressure range up to 2.39 GPa suggesting a reduction of the easy-axis type magnetocrystalline anisotropy energy (MAE). A quantitative analysis of the FMR data gives evidence that up to this pressure the MAE constant $K_{\rm U}$, although getting significantly smaller, still remains finite and positive, i.e. of the easy-axis type. Therefore, a recently discussed possibility of switching the sign of the magnetocrystalline anisotropy in Cr$_2$Ge$_2$Te$_6$ could only be expected at still higher pressures, if possible at all due to the observed weakening of the ferromagnetism under pressure. This circumstance may be of relevance for the design of strain-engineered functional heterostructures containing layers of Cr$_2$Ge$_2$Te$_6$.
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.
The van der Waals ferromagnet Fe5GeTe2 has a Curie temperature TC of about 270 K, which can be raised above room temperature by tuning the Fe deficiency content. To achieve insights into its ferromagnetic exchange, we have studied the critical behavior by measuring the magnetization in bulk Fe5GeTe2 crystal around the ferromagnetic to paramagnetic phase transition. The analysis of the magnetization by employing various techniques including the modified Arrott plot, Kouvel-Fisher plot and critical isotherm analysis achieved a set of reliable critical exponents with TC = 273.7 K, beta = 0.3457, …
The layered van der Waals ferromagnetic Fe$_3$GeTe$_2$ harbours an unconventional interplay between topology and magnetism, leading to a large anomalous Hall conductivity at low temperatures. Here, we investigate the temperature dependence of its charge dynamics and reveal that upon entering the ferromagnetic state at $T_C \sim 200$ K and further lowering the temperature there is the onset of a gradual spectral weight reshuffling from the mid-infrared range towards far- as well as near-infrared frequencies. This two-fold spectral weight transfer indicates the important role of the Hund's coupl…
Magnetoelastic coupling and uniaxial pressure dependencies of the ferromagnetic ordering temperature in the quasi-two-dimensional layered van-der-Waals material CrI$_3$ are experimentally studied and quantified by high-resolution dilatometry. Clear anomalies in the thermal expansion coefficients at $T_{\rm C}$ imply positive (negative) pressure dependencies $\partial T_{\rm C}/\partial p_{\rm i}$ for pressure applied along (perpendicular to) the $c$ axis. The experimental results are backed up by numerical studies showing that the dominant, intra-layer magnetic coupling increases upon compress…
We present a combined study of zero-field $^{51}$V and $^{127}$I NMR at ambient pressure and specific heat and magnetization measurements under pressure up to 2.08 GPa on bulk single crystals of the van-der-Waals ferromagnet VI$_3$. At ambient pressure, our results consistently demonstrate that VI$_3$ undergoes a structural transition at $T_s \approx $78 K, followed by two subsequent ferromagnetic transitions at $T_{FM1} \approx $50 K and $T_{FM2} \approx $36 K upon cooling. At lowest temperature ($T < T_{FM2}$), two magnetically-ordered V sites exist, whereas only one magnetically-ordered V s…
Van der Waals (vdW) ferromagnets are an important class of materials for spintronics applications. The recent discovery of atomically vdW magnets CrI$_3$ and Cr$_2$Ge$_2$Te$_6$ has triggered a renaissance in the area of two-dimensional (2D) magnetism. Herein we systematically studied 2H-Mn$_{0.28}$TaS$_2$ single crystal, a 2D vdW ferromagnet with $T_c$ $\sim$ 82.3 K and a large in-plane magnetic anisotropy. Mn $K$-edge x-ray absorption spectroscopy was measured to provide information on its electronic state and local atomic environment. The detailed magnetic isotherms measured in the vicinity …
The results of a single-crystal X-ray-diffraction study of the evolution of crystal structures of VI3 with temperature with emphasis on phase transitions are presented. Some related specific-heat and magnetization data are included. The existence of the room-temperature trigonal crystal structure R-3 (148) has been confirmed. Upon cooling, VI3 undergoes a structural phase transition to a monoclinic phase at Ts ~ 79 K. Ts is reduced in magnetic fields applied along the trigonal c-axis. When VI3 becomes ferromagnetic at TFM1 ~ 50 K, magnetostriction-induced changes of the monoclinic-structure pa…
We report anomalous Hall effect (AHE) in single crystals of quasi-two-dimensional Fe$_{3-x}$GeTe$_2$ ($x \approx 0.36$) ferromagnet grown by the flux method which induces defects on Fe site and bad metallic resistivity. Fe K-edge x-ray absorption spectroscopy was measured to provide information on local atomic environment in such crystals. The dc and ac magnetic susceptibility measurements indicate a second-stage transition below 119 K in addition to the paramagnetic to ferromagnetic transition at 153 K. A linear scaling behavior between the modified anomalous Hall resistivity $ρ_{xy}/μ_0H_{ef…
Thermal and Magnetoelastic Properties of the van der Waals Ferromagnet Fe$_{3-δ}$GeTe$_2$: Anisotropic Spontaneous Magnetostriction and Ferromagnetic Magnon Excitations
Two dimensional van der Waals ferromagnets with honeycomb structures are expected to host the bosonic version of Dirac particles in their magnon excitation spectra. Using inelastic neutron scattering, we study spin wave excitations in polycrystalline CrCl$_3$, which exhibits ferromagnetic honeycomb layers with antiferromagnetic stackings along the $c$-axis. For comparison, polycrystal samples of CrI$_3$ with different grain sizes are also studied. We find that the powder-averaged spin wave spectrum of CrCl$_3$ at $T$ = 2 K can be adequately explained by the two dimensional spin Hamiltonian inc…
We have grown a series of nickel substituted single crystals of the layered ferromagnet (FM) Fe$_3$GeTe$_2$. The large single crystalline samples of (Fe$_{1-x}$Ni$_x$)$_3$GeTe$_2$ with $x = 0-0.84$ were characterized with single crystal X-ray diffraction, magnetic susceptibility, electrical resistance and muon spin spectroscopy. We find Fe can be continuously substituted with Ni with only minor structural variation. In addition, FM order is suppressed from $T_\mathrm{C}=212$~K for $x=0$ down to $T_\mathrm{C}=50$~K for $x=0.3$, which is accompanied with a strong suppression of saturated and eff…
Ferromagnetic van der Waals (vdW) insulators are of great scientific interest for their promising applications in spintronics. It has been indicated that in the two materials within this class, CrI$_3$ and VI$_3$, the magnetic ground state, the band gap, and the Fermi level could be manipulated by varying the layer thickness, strain or doping. To understand how these factors impact the properties, a detailed understanding of the electronic structure would be required. However, the experimental studies of the electronic structure of these materials are still very sparse. Here, we present the de…
We have studied the magnetic properties of quasi two-dimensional itinerant ferromagnet Fe$_4$GeTe$_2$ as functions of temperature and magnetic field ($B$) with field parallel to the $ab$-plane ($B\|ab$) and $c$-axis ($B\|c$) of the crystal. This van der Waals compound undergoes a continuous paramagnetic to ferromagnetic phase transition below $T_C$ = 270.0 K and a pronounced spin reorientation transition at around $T_{SR}$ $\sim$ 115 K where the easy axis of magnetization changes its direction from in-plane to out-of-plane. The temperature evolution of magnetization in the FM state is highly a…
The critical properties of the single-crystalline van der Waals bonded ferromagnet Fe$_{3-x}$GeTe$_2$ were investigated by bulk dc magnetization around the paramagnetic (PM) to ferromagnetic (FM) phase transition. The Fe$_{3-x}$GeTe$_2$ single crystals grown by self-flux method with Fe deficiency $x \approx 0.36$ exhibit bulk FM ordering below $T_c = 152$ K. The Mössbauer spectroscopy was used to provide information on defects and local atomic environment in such crystals. Critical exponents $β= 0.372(4)$ with a critical temperature $T_c = 151.25(5)$ K and $γ= 1.265(15)$ with $T_c = 151.17(12)…
We theoretically propose a second-order topological magnon insulator by stacking the van der Waals honeycomb ferromagnets with antiferromagnetic interlayer coupling. The system exhibits Z$_{2}$ topological phase, protected by pseudo-time-reversal symmetry (PTRS). An easy-plane anisotropy term breaks PTRS and destroys the topological phase. Nevertheless, it respects a magnetic two-fold rotational symmetry which protects a second-order topological phase with corner modes in bilayer and hinge modes along stacking direction. Moreover, an introduced staggered interlayer coupling establishes a Z$_{2…
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…
Spin-reorientation as a switch for electronic topology in van der Waals ferromagnets
Indian Association for the Cultivation of Science（印度科学文化协会）；S. N. Bose National Centre for Basic Sciences（S.N. 玻色基础科学国家中心）；Saha Institute of Nuclear Physics, A CI of Homi Bhabha National Institute（萨哈核物理研究所（霍米·巴巴国立学院成员））；National Institute of Science Education and Research（国家科学教育研究中心）
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 a comprehensive experimental investigation on the magnetic anisotropy in bulk single crystals of Cr$_2$Ge$_2$Te$_6$, a quasi-two-dimensional ferromagnet belonging to the family of magnetic layered transition metal trichalcogenides that have attracted recently a big deal of interest with regard to the fundamental and applied aspects of two-dimensional magnetism. For this purpose electron spin resonance (ESR) and ferromagnetic resonance (FMR) measurements have been carried out over a wide frequency and temperature range. A gradual change in the angular dependence of the ESR linewidth a…
We report structural, physical properties and electronic structure of van der Waals (vdW) crystal VI3. Detailed analysis reveals that VI3 exhibits a structural transition from monoclinic C2/m to rhombohedral R-3 at Ts ~ 79 K, similar to CrX3 (X = Cl, Br, I). Below Ts, a long-range ferromagnetic (FM) transition emerges at Tc ~ 50 K. The local moment of V in VI3 is close to the high-spin state V3+ ion (S = 1). Theoretical calculation suggests that VI3 may be a Mott insulator with the band gap of about 0.84 eV. In addition, VI3 has a relative small interlayer binding energy and can be exfoliated …
Van der Waals magnet VI$_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 …
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…
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 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…
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）
In the new van der Waals Kondo-lattice Fe$_3$GeTe$_2$, itinerant ferromagnetism and heavy fermionic behaviour coexist. Both the key properties of such a system namely a spin-polarized Fermi surface and a low Fermi momentum are expected to significantly alter Andreev reflection dominated transport at a contact with a superconducting electrode, and display unconventional proximity-induced superconductivity. We observed interplay between Andreev reflection and Kondo resonance at mesoscopic interfaces between superconducting Nb and Fe$_3$GeTe$_2$. Above the critical temperature ($T_c$) of Nb, the …
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…
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…
Magnetic skyrmions in 2D chiral magnets are in general stabilized by a combination of Dzyaloshinskii-Moriya interaction and external magnetic field. Here, we show that skyrmions can also be stabilized in twisted moiré superlattices in the absence of an external magnetic field. Our setup consists of a 2D ferromagnetic layer twisted on top of an antiferromagnetic substrate. The coupling between the ferromagnetic layer and the substrate generates an effective alternating exchange field. We find a large region of skyrmion crystal phase when the length scales of the moiré periodicity and skyrmions …
Twisted van der Waals materials have become a paradigmatic platform to realize exotic correlated states of matter. Here, we show that a twisted dichalcogenide bilayer (WSe$_2$) encapsulated between a magnetic van der Waals material (CrBr$_3$) features flat bands with tunable valley and spin flavors. We demonstrate that, when electron-electron interactions are included, spin-ferromagnetic and valley-ferromagnetic states emerge in the flat bands, stemming from the interplay between correlations, intrinsic spin-orbit coupling and exchange proximity effects. We show that the specific symmetry brok…
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）
Fe$_{5-x}$GeTe$_2$ is a centrosymmetric, layered van der Waals (vdW) ferromagnet that displays Curie temperatures $T_c$ (270-330 K) that are within the useful range for spintronic applications. However, little is known about the interplay between its topological spin textures (e.g., merons, skyrmions) with technologically relevant transport properties such as the topological Hall effect (THE), or topological thermal transport. Here, we show via high-resolution Lorentz transmission electron microscopy that merons and anti-meron pairs coexist with Néel skyrmions in Fe$_{5-x}$GeTe$_2$ over a wide…
