Magnetic field-induced quantum phase transitions in a van der Waals magnet
Siwen Li, Zhipeng Ye, Xiangpeng Luo, Gaihua Ye, Hyun Ho Kim, Bowen Yang, Shangjie Tian, Chenghe Li, Hechang Lei, Adam W. Tsen, Kai Sun, Rui He, Liuyan Zhao
Exploring new parameter regimes to realize and control novel phases of matter has been a main theme in modern condensed matter physics research. The recent discovery of 2D magnetism in nearly freestanding monolayer atomic crystals has already led to observations of a number of novel magnetic phenomena absent in bulk counterparts. Such intricate interplays between magnetism and crystalline structures provide ample opportunities for exploring quantum phase transitions in this new 2D parameter regime. Here, using magnetic field and temperature dependent circularly polarized Raman spectroscopy of phonons and magnons, we map out the phase diagram of CrI3 that has been known to be a layered AFM in its 2D films and a FM in its 3D bulk. We, however, reveal a novel mixed state of layered AFM and FM in 3D CrI3 bulk crystals where the layered AFM survives in the surface layers and the FM appears in deeper bulk layers. We then show that the surface layered AFM transits into the FM at a critical magnetic field of 2 T, similar to what was found in the few layer case. Interestingly, concurrent with this magnetic phase transition, we discover a first-order structural phase transition that alters the crystallographic point group from C3i to C2h and thus, from a symmetry perspective, this monoclinic structural phase belongs to the 3D nematic order universality class. Our result not only unveils the complex single magnon behavior in 3D CrI3, but also settles down the puzzle of how CrI3 transits from a bulk FM to a thin layered AFM semiconductor, despite recent efforts in understanding the origin of layered AFM in CrI3 thin layer, and reveals the intimate relationship between the layered AFM-to-FM and the crystalline rhombohedral-to-monoclinic phase transitions. These findings further open up opportunities for future 2D magnet-based magneto-mechanical devices.
The recent emergence of 2D van der Waals magnets down to atomic layer thickness provides an exciting platform for exploring quantum magnetism and spintronics applications. The van der Waals nature stabilizes the long-range ferromagnetic order as a result of magnetic anisotropy. Furthermore, giant tunneling magnetoresistance and electrical control of magnetism have been reported. However, the potential of 2D van der Waals magnets for magnonics, magnon-based spintronics, has not been explored yet. Here, we report the experimental observation of long-distance magnon transport in quasi-twodimensio…
We present a phenomenological theory for coupled spin-charge dynamics in magnetic van der Waals heterostructures. The system studied consists of a layered antiferromagnet inserted into a capacitive vdW heterostructure. It has been recently demonstrated that charge doping in such layered antiferromagnets can modulate the strength, and even the sign, of exchange coupling between the layer magnetizations. This provides a mechanism for electrically generating magnetization dynamics. The central result we predict here is that the magnetization dynamics reciprocally results in inducing charge dynami…
Due to the atomically thin nature of monolayer and few-layer van der Waals magnets, the undesired background signal from the substrate can have significant contribution when characterizing their magnetic properties. This brings challenges in accurately determining the magnitude of the magnetic moment of the epitaxially grown van der Waals magnets on bulk substrates. In this paper, we discuss the impact of the background subtraction method for accurately determining the magnetic moments in such systems. Using the recently reported intrinsic two-dimensional (2D) van der Waals ferromagnet MnSe${_…
Multiple magnetic skyrmion phases add an additional degree of freedom for skyrmion based ultrahigh-density spin memory devices. Extending the field to two-dimensional van der Waals magnets is a rewarding challenge, where the realizable degree of freedoms (e.g. thickness, twisting angle and electrical gating) and high skyrmion density result in intriguing new properties and enhanced functionality. We report a van der Waals interface, formed by two 2D ferromagnets Cr2Ge2Te6 and Fe3GeTe2 with a Curie temperature of ~65 K and ~205 K, respectively, hosting two groups of magnetic skyrmions. Two sets…
Using bilayer CrI$_3$ as an example, we demonstrate that stacking domain walls in van der Waals magnets can host one dimensional (1D) magnon channels, which have lower energies than bulk magnons. Interestingly, some magnon channels are hidden in magnetically homogeneous background and can only be inferred with the knowledge of stacking domain walls. Compared to 1D magnons confined in magnetic domain walls, 1D magnons in stacking domain walls are more stable against external perturbations. We show that the relaxed moiré superlattices of small-angle twisted bilayer CrI$_3$ is a natural realizati…
There has been a huge increase of interests in two-dimensional van der Waals materials over the past ten years or so with the conspicuous absence of one particular class of materials: magnetic van der Waals systems. In this Viewpoint, we point it out and illustrate how we might be able to benefit from exploring these so-far neglected materials.
Experimental demonstrations of 1D van der Waals material tellurium have been presented by Raman spectroscopy under strain and magneto-transport. Raman spectroscopy measurements have been performed under strains along different principle axes. Pronounced strain response along c-axis is observed due to the strong intra-chain covalent bonds, while no strain response is obtained along a-axis due to the weak inter-chain van der Waals interaction. Magneto-transport results further verify its anisotropic property, resulting in dramatically distinct magneto-resistance behaviors in terms of three diffe…
Spin-waves have been studied for data storage, communication and logic circuits in the field of spintronics based on their potential to substitute electrons. Recent discovery of magnetism in two-dimensional (2D) systems such as monolayer CrI$_3$ and Cr$_2$Ge$_2$Te$_6$ has led to a renewed interest in such applications of magnetism in the 2D limit. Here we present direct evidence of standing spin-waves along with the uniform precessional resonance modes in van der Waals magnetic material, CrCl$_3$. Our experiment is the first direct observation of standing spin-wave modes, set up across a thick…
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…
We investigate the magnetic proximity effect in van der Waals heterostructure formed by a monolayer semiconductor stacked on a 2D ferromagnet, where the lattice mismatch and twisting between the layers typically lead to the formation of moiré pattern. We find that the magnetic proximity effect arising from the spin dependent interlayer coupling depends sensitively on the interlayer atomic registry. Consequently, in the moiré pattern, the spatial variation of the atomic registry leads to a lateral modulation of magnetic proximity field. Such moiré modulated magnetic proximity effect manifests a…
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…
Atomically thin chromium triiodide (CrI3) has recently been identified as a layered antiferromagnetic insulator, in which adjacent ferromagnetic monolayers are antiferromagnetically coupled. This unusual magnetic structure naturally comprises a series of anti-aligned spin filters which can be utilized to make spin-filter magnetic tunnel junctions with very large tunneling magnetoresistance (TMR). Here we report voltage control of TMR formed by four-layer CrI3 sandwiched by monolayer graphene contacts in a dual-gated structure. By varying the gate voltages at fixed magnetic field, the device ca…
Van der Waals magnets are uniquely positioned at the intersection between two-dimensional materials, antiferromagnetic spintronics, and magnonics. The interlayer exchange interaction in these materials enables antiferromagnetic resonances to be accessed at GHz frequencies. Consequently, these layered antiferromagnets are intriguing materials out of which quantum hybrid magnonic devices can be fashioned. Here, we use both a modified macrospin model and micromagnetic simulations to demonstrate a comprehensive antiferromagnetic resonance spectra in van der Waals magnets near the ultrathin (monola…
The magnetic tunnel junction (MTJ) is a backbone device for spintronics. Realizing next generation energy efficient MTJs will require operating mechanisms beyond the standard means of applying magnetic fields or large electrical currents. Here, we demonstrate a new concept for programmable MTJ operation via strain control of the magnetic states of CrSBr, a layered antiferromagnetic semiconductor used as the tunnel barrier. Switching the CrSBr from antiferromagnetic to ferromagnetic order generates a giant tunneling magnetoresistance ratio without external magnetic field at temperatures up to ~…
Spin-dependent transport in a full van der Waals (vdW) giant magnetoresistance (GMR) junctions with the structure of Fe3GeTe2/XTe2/Fe3GeTe2 (X = Pt, Pd) has been investigated by using first-principles calculations. The ballistic conductance, magnetoresistance (MR) and resistance-area product (RA) have been calculated in a current-perpendicular-to-plane (CPP) geometry. A giant magnetoresistance of around 2000% and RA less than 0.3 Ω μm2 have been found in the proposed vdW CPP GMR. In addition, the spin-orbit coupling effect on transport and anisotropy magnetoresistance (AMR) has also been inves…
Manipulating quantum state via electrostatic gating has been intriguing for many model systems in nanoelectronics. When it comes to the question of controlling the electron spins, more specifically, the magnetism of a system, tuning with electric field has been proven to be elusive. Recently, magnetic layered semiconductors have attracted much attention due to their emerging new physical phenomena. However, challenges still remain in the demonstration of a gate controllable magnetism based on them. Here, we show that, via ionic gating, strong field effect can be observed in few-layered semicon…
We study the microscopical origin of anisotropic ferromagnetism in the van der Waals magnet CrI3. We conclude that the nearest neighbors exchange is well described by the Heisenberg-Kitaev-Gamma (HKGamma) model, and we also found a nonzero Dzyaloshinskii-Moriya interaction (DMI) on next nearest neighbors. Both Kitaev and DMI are known to generate a non-trivial topology of the magnons in the honeycomb lattice and have been used separately to describe the low energy regime of this material. We discuss that including one or the other leads to different signs of the Chern number. Furthermore, the …
The development of van der Waals (vdW) crystals and their heterostructures has created a fascinating platform for exploring optoelectronic properties in the two-dimensional (2D) limit. With the recent discovery of 2D magnets, the control of the spin degree of freedom can be integrated to realize 2D spin-optoelectronics with spontaneous time-reversal symmetry breaking. Here, we report spin photovoltaic effects in vdW heterostructures of atomically thin magnet chromium triiodide (CrI3) sandwiched by graphene contacts. In the absence of a magnetic field, the photocurrent displays a distinct depen…
Strain Tuning of Orbital-Driven Giant Magnetoresistance in van der Waals ferrimagnet Mn$_3$Si$_2$Te$_6$
Institute for Solid State Physics, The University of Tokyo（东京大学固体离子体研究所）；The University of Tokyo（东京大学）；Department of Physics and Astronomy, The University of Manchester（曼彻斯特大学物理与天文学系）；The University of Manchester（曼彻斯特大学）；Department of Physics, Institute of Science Tokyo（东京科学大学物理系）；Institute of Science Tokyo（东京科学大学）
Magnetic van der Waals materials provide an ideal playground for exploring the fundamentals of low-dimensional magnetism and open new opportunities for ultrathin spin processing devices. The Mermin-Wagner theorem dictates that as in reduced dimensions isotropic spin interactions cannot retain long-range correlations; the order is stabilized by magnetic anisotropy. Here, using ultrashort pulses of light, we demonstrate all-optical control of magnetic anisotropy in the two-dimensional van der Waals antiferromagnet NiPS$_3$. Tuning the photon energy in resonance with an orbital transition between…
Geometry-Controlled Magnetic and Electronic Landscapes in Anisotropic van der Waals Materials
Wroclaw University of Science and Technology（弗罗茨瓦夫理工大学）；University of Warsaw（华沙大学）；Wrocław University of Science and Technology（弗罗茨瓦夫理工大学）；University of Chemistry and Technology Prague（布拉格化工大学）
In recent years, noncollinear topological textures have long gained increasing research attentions for their high values of both fundamental researches and potential applications. The recent discovery of intrinsic orders in magnetic and polar two-dimensional van der Waals materials provides a new ideal platform for the investigation of noncollinear topological textures. Here, we review the theoretical and experimental progresses on noncollinear topological textures in two-dimensional van der Waals materials in very recent years. During these years, magnetic skyrmions of both Bloch and Néel typ…
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…
We report the observation of a very large negative magnetoresistance effect in a van der Waals tunnel junction incorporating a thin magnetic semiconductor, CrI3, as the active layer. At constant voltage bias, current increases by nearly one million percent upon application of a 2 Tesla field. The effect arises from a change between antiparallel to parallel alignment of spins across the different CrI3 layers. Our results elucidate the nature of the magnetic state in ultrathin CrI3 and present new opportunities for spintronics based on two-dimensional materials.
We report the isolation of thin flakes of cylindrite, a naturally occurring van der Waals superlattice, by means of mechanical and liquid phase exfoliation. We find that this material is a heavily doped p-type semiconductor with a narrow gap (<0.85 eV) with intrinsic magnetic interactions that are preserved even in the exfoliated nanosheets. Due to its environmental stability and high electrical conductivity, cylindrite can be an interesting alternative to the existing two-dimensional magnetic materials.
Multiferroic materials with coupled ferroelectric and ferromagnetic properties are important for multifunctional devices due to their potential ability of controlling magnetism via electric field, and vice versa. The recent discoveries of two-dimensional ferromagnetic and ferroelectric materials have ignited tremendous research interest and aroused hope to search for two-dimensional multiferroics. However, intrinsic two-dimensional multiferroic materials and, particularly, those with strong magnetoelectric couplings are still rare to date. In this paper, using first-principles simulations, we …
Heterostructures having both magnetism and topology are promising materials for the realization of exotic topological quantum states while challenging in synthesis and engineering. Here, we report natural magnetic van der Waals heterostructures of (MnBi2Te4)m(Bi2Te3)n that exhibit controllable magnetic properties while maintaining their topological surface states. The interlayer antiferromagnetic exchange coupling is gradually weakened as the separation of magnetic layers increases, and an anomalous Hall effect that is well coupled with magnetization and shows ferromagnetic hysteresis was obse…
In layered magnetic materials, the magnetic coupling between neighboring van der Waals layers is challenging to understand and anticipate, although the exchange interaction inside a layer can be well rationalized for example by the superexchange mechanism. In this work, we elucidate the interlayer exchange mechanism and propose an electron-counting rule to determine the interlayer magnetic order between van der Waals layers, based on counting the $d$-orbital occupation ($d^n$, where $n$ is the number of $d$-electrons at the magnetic cation). With this rule, we classify magnetic monolayers into…
Demonstration of room-temperature, magnetic-field-free, and ultralow-power spin-orbit torque logic device based on composition-uniform van der Waals magnet Fe3GaTe2
State Key Laboratory of Semiconductor Physics and Chip Technologies, Institute of Semiconductors, Chinese Academy of Sciences（中国科学院半导体研究所）；Center of Materials Science and Optoelectronics Engineering, University of Chinese Academy of Sciences（中国科学院大学）；College of Physics and Information Technology, Shaanxi Normal University（陕西师范大学物理与信息工程学院）
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…
Electrical control of magnetism in a two-dimensional (2D) semiconductor is of great interest for emerging nanoscale low-dissipation spintronic devices. Here, we propose a general approach of tuning magnetic coupling and anisotropy of a van der Waals (vdW) 2D magnetic semiconductor via a built-in electric field generated by the adsorption of superatomic ions. Using first-principles calculations, we predict a significant enhancement of ferromagnetic (FM) coupling and a great change of magnetic anisotropy in 2D semiconductors when they are sandwiched between superatomic cations and anions. The ma…
Magnetic van der Waals (vdW) materials, including ferromagnets (FM) and antiferromagnets (AFM), have given access to the investigation of magnetism in two-dimensional (2D) limit and attracted broad interests recently. However, most of them are semiconducting or insulating and the vdW itinerant magnets, especially vdW itinerant AFM, are very rare. Here, we studied the anomalous Hall effect of a vdW itinerant magnet Fe$_5$GeTe$_2$ (F5GT) with various thicknesses down to 6.8 nm (two unit cells). Despite the robust ferromagnetic ground state in thin-layer F5GT, however, we show that the electron d…
Manipulating the interlayer magnetic coupling in van der Waals magnetic materials and heterostructures is the key to tailoring their magnetic and electronic properties for various electronic applications and fundamental studies in condensed matter physics. By utilizing the MnBi2Te4-family compounds and their heterostructures as a model system, we systematically studied the dependence of the sign and strength of interlayer magnetic coupling on constituent elements by using first-principles calculations. It was found that the coupling is a long-range superexchange interaction mediated by the cha…
The exfoliation of two naturally occurring van der Waals minerals, graphite and molybdenite, arouse an unprecedented level of interest by the scientific community and shaped a whole new field of research: 2D materials research. Several years later, the family of van der Waals materials that can be exfoliated to isolate 2D materials keeps growing, but most of them are synthetic. Interestingly, in nature plenty of naturally occurring van der Waals minerals can be found with a wide range of chemical compositions and crystal structures whose properties are mostly unexplored so far. This Perspectiv…
Precision magnetometry is fundamental to the development of novel magnetic materials and devices. Recently, the nitrogen-vacancy (NV) center in diamond has emerged as a promising probe for static magnetism in 2D van der Waals materials, capable of quantitative imaging with nanoscale spatial resolution. However, the dynamic character of magnetism, crucial for understanding the magnetic phase transition and achieving technological applications, has rarely been experimentally accessible in single 2D crystals. Here, we coherently control the NV center's spin precession to achieve ultra-sensitive, …
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 …
Magnetic insulators are a key resource for next-generation spintronic and topological devices. The family of layered metal halides promises ultrathin insulating multiferroics, spin liquids, and ferromagnets, but new characterization methods are required to unlock their potential. Here, we report tunneling through the layered magnetic insulator CrI3 as a function of temperature and applied magnetic field. We electrically detect the magnetic ground state and inter-layer coupling and observe a field-induced metamagnetic transition. The metamagnetic transition results in magnetoresistances of 95%,…
In two-dimensional (2D) magnetic systems, large magnetic anisotropy is needed to stabilize the magnetic order according to Mermin-Wagner theorem. Based on density functional theory (DFT) calculations, we propose that the magnetic anisotropic energy (MAE) of 2D ferromagnetic (FM) semiconductors can be strongly enhanced in van der Waals heterostructures by attaching a nonmagnetic semiconductor monolayer with large spin-orbit coupling. We studied Cr2Ge2Te6/PtSe2 bilayer heterostructures, where each layer has been realized in recent experiments. The DFT calculations show that the MAE of Cr2Ge2Te6/…
Van der Waals (vdW) heterostructures have attracted great interest because of their rich material combinations.The discovery of two-dimensional magnets has provided a new platform for magnetic vdW heterointerfaces; however, research on magnetic vdW heterointerfaces has been limited to those with ferromagnetic surfaces. Here we report a magnetic vdW heterointerface using layered intralayer-antiferromagnetic MPSe3 (M=Mn, Fe) and monolayer transition metal dichalcogenides (TMDs). We found an anomalous upshift of the excitonic peak in monolayer TMDs below the antiferromagnetic transition temperatu…
Activating metamagnetic transitions between ordered states in van der Waals magnets and devices bring great opportunities in spintronics. We show that external pressure, which enhances the interlayer hopping without introducing chemical disorders, triggers multiple metamagnetic transitions upon cooling in the topological van der Waals magnets Mn(Bi$_{1-x}$Sb$_x$)$_4$Te$_7$, where the antiferromagnetic interlayer superexchange coupling competes with the ferromagnetic interlayer coupling mediated by the antisite Mn spins. The temperature-pressure phase diagrams reveal that while the ordering tem…
Incorporating magnetism into two dimensional (2D) van der Waals (VdW) heterostrutures is crucial for the development of functional electronic and magnetic devices. Here we show that Nb3X8 (X = Cl, Br) is a family of 2D layered trimerized kagomé magnets that are paramagnetic at high temperatures and undergo a first order phase transition on cooling to a singlet magnetic state. X-ray diffraction shows that a rearrangement of the VdW stacking accompanies the magnetic transition, with high and low temperature phases consistent with STEM images of the end members α-Nb3Cl8 and \b{eta}-Nb3Br8. The te…
We propose a tubal van der Waals heterostructure by rolling up the graphene and MoS2 atomic layers into a tubal form. We illustrate that the interlayer space for the tubal van der Waals heterostructure can be varied in a specific range, which is determined by the competition between the interlayer van der Waals force and the mechanical properties of the atomic layers. The variability of the interlayer space can be utilized to efficiently tune mechanical properties of the tubal van der Waals heterostructure. More specifically, we demonstrate that the Poisson's ratio of the tubal van der Waals h…
Recent developments in two-dimensional (2D) magnetism have motivated the search for novel van-der Waals (vdWs) magnetic materials to explore new magnetic phenomenon in the 2D limit. Metal thiophosphates, MPX3, is a class of magnetic vdWs materials with antiferromagnetic (AFM) ordering persisting down to the atomically thin limit. The magnetism in this material family has been found to be highly dependent on the choice of transition metal M. In this work, we have synthesized the intermediate compounds Ni1-xMnxPS3 (0 < x < 1) and investigated their magnetic properties. Our study reveals that the…
Spontaneous magnetic order is a routine instance in three-dimensional (3D) materials but for a long time, it remained elusive in the 2D world. Recently, the first examples of (stand-alone) 2D van der Waals (vdW) crystals with magnetic order, either antiferromagnetic or ferromagnetic, have been reported. In this review, we describe the state of the art of the nascent field of magnetic 2D materials focusing on synthesis, engineering, and theory aspects. We also discuss challenges and some of the many different promising directions for future work.
Discovery of Van Hove Singularities: Electronic Fingerprints of 3Q Magnetic Order in a van der Waals Quantum Magnet
University of California, Berkeley（加州大学伯克利分校）；Lawrence Berkeley National Laboratory（劳伦斯伯克利国家实验室）；Nanyang Technological University（南洋理工大学）；CIFAR（加拿大联邦先进研究基金会）；Kavli Energy NanoScience Institute（卡弗里能源纳米科学研究所）
