Showing papers on "Antiferromagnetism published in 2019"

Experimental Realization of an Intrinsic Magnetic Topological Insulator

Abstract: An intrinsic magnetic topological insulator (TI) is a stoichiometric magnetic compound possessing both inherent magnetic order and topological electronic states. Such a material can provide a shortcut to various novel topological quantum effects but remained elusive experimentally for a long time. Here we report the experimental realization of thin films of an intrinsic magnetic TI, MnBi 2 Te 4 , by alternate growth of a Bi 2 Te 3 quintuple layer and a MnTe bilayer with molecular beam epitaxy. The material shows the archetypical Dirac surface states in angle-resolved photoemission spectroscopy and is demonstrated to be an antiferromagnetic topological insulator with ferromagnetic surfaces by magnetic and transport measurements as well as first-principles calculations. The unique magnetic and topological electronic structures and their interplays enable the material to embody rich quantum phases such as quantum anomalous Hall insulators and axion insulators at higher temperature and in a well-controlled way.

Magnetic-field-induced quantized anomalous Hall effect in intrinsic magnetic topological insulator MnBi$_2$Te$_4$

Abstract: In a magnetic topological insulator, nontrivial band topology conspires with magnetic order to produce exotic states of matter that are best exemplified by quantum anomalous Hall (QAH) insulators and axion insulators. Up till now, such magnetic topological insulators are obtained by doping topological insulators with magnetic atoms. The random magnetic dopants, however, inevitably introduce disorders that hinder further exploration of quantum effects in the material. Here, we resolve this dilemma by probing quantum transport in MnBi$_2$Te$_4$ thin flake - a topological insulator with intrinsic magnetic order. In this layered van der Waals crystal, the ferromagnetic layers couple anti-parallel to each other, so MnBi$_2$Te$_4$ is an antiferromagnet. A magnetic field, however, aligns all the layers and induces an interlayer ferromagnetic order; we show that a quantized anomalous Hall response emerges in atomically thin MnBi$_2$Te$_4$ under a moderate magnetic field. MnBi$_2$Te$_4$ therefore becomes the first intrinsic magnetic topological insulator exhibiting quantized anomalous Hall effect. The result establishes MnBi$_2$Te$_4$ as an ideal arena for further exploring various topological phenomena.

Direct observation of van der Waals stacking dependent interlayer magnetism

Abstract: Controlling the crystal structure is a powerful approach for manipulating the fundamental properties of solids. Unique to two-dimensional (2D) van der Waals materials, the control can be achieved by modifying the stacking order through rotation and translation between the layers. Here, we report the first observation of stacking dependent interlayer magnetism in the 2D magnetic semiconductor, chromium tribromide (CrBr3), enabled by the successful growth of its monolayer and bilayer through molecular beam epitaxy. Using in situ spin-polarized scanning tunneling microscopy and spectroscopy, we directly correlated the atomic lattice structure with observed magnetic order. We demonstrated that while individual CrBr3 monolayer is ferromagnetic, the interlayer coupling in bilayer depends strongly on the stacking order and can be either ferromagnetic or antiferromagnetic. Our observations provide direct experimental evidence for exploring the stacking dependent layered magnetism, and pave the way for manipulating 2D magnetism with unique layer twist angle control.

Switching 2D magnetic states via pressure tuning of layer stacking

Abstract: The physical properties of two-dimensional van der Waals crystals can be sensitive to interlayer coupling. For two-dimensional magnets1–3, theory suggests that interlayer exchange coupling is strongly dependent on layer separation while the stacking arrangement can even change the sign of the interlayer magnetic exchange, thus drastically modifying the ground state4–10. Here, we demonstrate pressure tuning of magnetic order in the two-dimensional magnet CrI3. We probe the magnetic states using tunnelling8,11–13 and scanning magnetic circular dichroism microscopy measurements2. We find that interlayer magnetic coupling can be more than doubled by hydrostatic pressure. In bilayer CrI3, pressure induces a transition from layered antiferromagnetic to ferromagnetic phase. In trilayer CrI3, pressure can create coexisting domains of three phases, one ferromagnetic and two antiferromagnetic. The observed changes in magnetic order can be explained by changes in the stacking arrangement. Such coupling between stacking order and magnetism provides ample opportunities for designer magnetic phases and functionalities. Pressure-induced changes in the magnetic order of bilayer and trilayer van der Waals crystals are revealed and attributed to changes in the stacking arrangement.

Stacking-dependent magnetism in bilayer CrI3

Abstract: We report the connection between the stacking order and magnetic properties of bilayer CrI3 using first-principles calculations. We show that the stacking order defines the magnetic ground state. By changing the interlayer stacking order, one can tune the interlayer exchange interaction between antiferromagnetic and ferromagnetic. To measure the predicted stacking-dependent magnetism, we propose using linear magnetoelectric effect. Our results not only gives a possible explanation for the observed antiferromagnetism in bilayer CrI3 but also have direct implications in heterostructures made of two-dimensional magnets.

Probing magnetism in 2D materials at the nanoscale with single-spin microscopy.

Abstract: The discovery of ferromagnetism in two-dimensional (2D) van der Waals (vdW) crystals has generated widespread interest. Making further progress in this area requires quantitative knowledge of the magnetic properties of vdW magnets at the nanoscale. We used scanning single-spin magnetometry based on diamond nitrogen-vacancy centers to image the magnetization, localized defects, and magnetic domains of atomically thin crystals of the vdW magnet chromium(III) iodide (CrI3). We determined the magnetization of CrI3 monolayers to be ≈16 Bohr magnetons per square nanometer, with comparable values in samples with odd numbers of layers; however, the magnetization vanishes when the number of layers is even. We also found that structural modifications can induce switching between ferromagnetic and antiferromagnetic interlayer ordering. These results demonstrate the benefit of using single-spin scanning magnetometry to study the magnetism of 2D vdW magnets.

Giant and nonreciprocal second harmonic generation from layered antiferromagnetism in bilayer CrI3

Abstract: Layered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. Recently, the van der Waals magnet, chromium triiodide (CrI3), emerged as the first layered antiferromagnetic insulator in its few-layer form, opening up ample opportunities for novel device functionalities. Here, we discovered an emergent nonreciprocal second order nonlinear optical effect in bilayer CrI3. The observed second harmonic generation (SHG) is giant: several orders of magnitude larger than known magnetization induced SHG and comparable to SHG in the best 2D nonlinear optical materials studied so far (e.g. MoS2). We showed that while the parent lattice of bilayer CrI3 is centrosymmetric and thus does not contribute to the SHG signal, the observed nonreciprocal SHG originates purely from the layered antiferromagnetic order, which breaks both spatial inversion and time reversal symmetries. Furthermore, polarization-resolved measurements revealed the underlying C2h symmetry, and thus monoclinic stacking order in CrI3 bilayers, providing crucial structural information for the microscopic origin of layered antiferromagnetism. Our results highlight SHG as a highly sensitive probe that can reveal subtle magnetic order and open novel nonlinear and nonreciprocal optical device possibilities based on 2D magnets.

Stacking tunable interlayer magnetism in bilayer CrI 3

Abstract: Interlayer magnetic interactions between two-dimension van der Waals layers are often thought to be weak or even negligible and their mechanism is largely unexplored. Here, the authors propose a mechanism for these interactions in a CrI${}_{3}$ bilayer, based on the concept of covalent-like quasibonding, which offers significant alteration of interlayer wave-function hybridization but small energetic difference between different stacking configurations. While a near-collinear coupling between two parallel spin-polarized I 5$p$ orbitals prefers interlayer ferromagnetism, a noncollinear one favors antiferromagnetism, which is tunable by surmounting a tiny energy barrier between two stacking orders. This explains experimental observations and suggests a strategy for designing interlayer magnetism.

Magnetic and magnetic inverse spin Hall effects in a non-collinear antiferromagnet

Abstract: The spin Hall effect (SHE)1–5 achieves coupling between charge currents and collective spin dynamics in magnetically ordered systems and is a key element of modern spintronics6–9. However, previous research has focused mainly on non-magnetic materials, so the magnetic contribution to the SHE is not well understood. Here we show that antiferromagnets have richer spin Hall properties than do non-magnetic materials. We find that in the non-collinear antiferromagnet10 Mn3Sn, the SHE has an anomalous sign change when its triangularly ordered moments switch orientation. We observe contributions to the SHE (which we call the magnetic SHE) and the inverse SHE (the magnetic inverse SHE) that are absent in non-magnetic materials and that can be dominant in some magnetic materials, including antiferromagnets. We attribute the dominance of this magnetic mechanism in Mn3Sn to the momentum-dependent spin splitting that is produced by non-collinear magnetic order. This discovery expands the horizons of antiferromagnet spintronics and spin–charge coupling mechanisms. A magnetic contribution to the spin Hall effect is observed in the non-collinear antiferromagnet Mn3Sn, which is attributed to momentum-dependent spin splitting produced by non-collinear magnetic order.

Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS 3

Abstract: How a certain ground state of complex physical systems emerges, especially in two-dimensional materials, is a fundamental question in condensed-matter physics. A particularly interesting case is systems belonging to the class of XY Hamiltonian where the magnetic order parameter of conventional nature is unstable in two-dimensional materials leading to a Berezinskii−Kosterlitz−Thouless transition. Here, we report how the XXZ-type antiferromagnetic order of a magnetic van der Waals material, NiPS3, behaves upon reducing the thickness and ultimately becomes unstable in the monolayer limit. Our experimental data are consistent with the findings based on renormalization-group theory that at low temperatures a two-dimensional XXZ system behaves like a two-dimensional XY one, which cannot have a long-range order at finite temperatures. This work provides the experimental examination of the XY magnetism in the atomically thin limit and opens opportunities of exploiting these fundamental theorems of magnetism using magnetic van der Waals materials. Exploring the ground state of two-dimensional (2D) magnetic systems enriches the fundamental understanding of magnetism and boosts the applications. The authors here show the suppression of magnetic order and 2D XY behavior in XXZ-type antiferromagnet NiPS3 when approaching the monolayer limit by Raman spectroscopy.

Atomically Thin CrCl3: An In-Plane Layered Antiferromagnetic Insulator.

Abstract: The recent discovery of magnetism in atomically thin layers of van der Waals (vdW) crystals has created new opportunities for exploring magnetic phenomena in the two-dimensional (2D) limit. In most 2D magnets studied to date, the c-axis is an easy axis, so that at zero applied field the polarization of each layer is perpendicular to the plane. Here, we demonstrate that atomically thin CrCl3 is a layered antiferromagnetic insulator with an easy-plane normal to the c-axis, that is, the polarization is in the plane of each layer and has no preferred direction within it. Ligand-field photoluminescence at 870 nm is observed down to the monolayer limit, demonstrating its insulating properties. We investigate the in-plane magnetic order using tunneling magnetoresistance in graphene/CrCl3/graphene tunnel junctions, establishing that the interlayer coupling is antiferromagnetic down to the bilayer. From the temperature dependence of the magnetoresistance, we obtain an effective magnetic phase diagram for the bilayer. Our result shows that CrCl3 should be useful for studying the physics of 2D phase transitions and for making new kinds of vdW spintronic devices.

Robust axion insulator and Chern insulator phases in a two-dimensional antiferromagnetic topological insulator

Abstract: The intricate interplay between nontrivial topology and magnetism in two-dimensional (2D) materials has led to the emergence of many novel phenomena and functionalities. An outstanding example is the quantum anomalous Hall (QAH) effect, which was realized in magnetically doped topological insulators (TIs) in the absence of magnetic field. Recently, the layered van der Waals compound MnBi2Te4 has been theoretically predicted and experimentally verified to be a TI with interlayer antiferromagnetic (AFM) order. It is a rare stoichiometric material with coexisting topology and magnetism, thus represents a perfect building block for complex topological-magnetic structures. Here we investigate the quantum transport behaviors of both bulk crystal and exfoliated MnBi2Te4 flakes in a field effect transistor geometry. In the 6 septuple layers (SLs) device tuned into the insulating regime, we observe a large longitudinal resistance and zero Hall plateau, which are characteristic of the axion insulator state. The robust axion insulator state occurs in zero magnetic field, over a wide magnetic field range, and at relatively high temperatures. Moreover, a moderate magnetic field drives a quantum phase transition from the axion insulator phase to a Chern insulator phase with zero longitudinal resistance and quantized Hall resistance h/e2 (h is the Plank constant and e is the elemental charge). These results pave the road for using even-number-SL MnBi2Te4 to realize the quantized topological magnetoelectric effect and axion electrodynamics in condensed matter systems.

Dirac fermions and flat bands in the ideal kagome metal FeSn

Abstract: The kagome lattice based on 3d transition metals is a versatile platform for novel topological phases hosting symmetry-protected electronic excitations and exotic magnetic ground states. However, the paradigmatic states of the idealized two-dimensional (2D) kagome lattice - Dirac fermions and topological flat bands - have not been simultaneously observed, partly owing to the complex stacking structure of the kagome compounds studied to date. Here, we take the approach of examining FeSn, an antiferromagnetic single-layer kagome metal with spatially-decoupled kagome planes. Using polarization- and termination-dependent angle-resolved photoemission spectroscopy (ARPES), we detect the momentum-space signatures of coexisting flat bands and Dirac fermions in the vicinity of the Fermi energy. Intriguingly, when complemented with bulk-sensitive de Haas-van Alphen (dHvA) measurements, our data reveal an even richer electronic structure that exhibits robust surface Dirac fermions on specific crystalline terminations. Through band structure calculations and matrix element simulations, we demonstrate that the bulk Dirac bands arise from in-plane localized Fe-3d orbitals under kagome symmetry, while the surface state realizes a rare example of fully spin-polarized 2D Dirac fermions when combined with spin-layer locking in FeSn. These results highlight FeSn as a prototypical host for the emergent excitations of the kagome lattice. The prospect to harness these excitations for novel topological phases and spintronic devices is a frontier of great promise at the confluence of topology, magnetism, and strongly-correlated electron physics.

Spin scattering and noncollinear spin structure-induced intrinsic anomalous Hall effect in antiferromagnetic topological insulator MnB i 2 T e 4

Abstract: This paper shows a spin fluctuation-driven spin scattering and a metastable canted antiferromagnetic phase in MnBi${}_{2}$Te${}_{4}$. These are signatures of an intrinsic anomalous Quantum Hall effect and open up new avenues to realize a quantum anomalous Hall insulator at high temperatures

Direct observation of van der Waals stacking–dependent interlayer magnetism

Abstract: Controlling the crystal structure is a powerful approach for manipulating the fundamental properties of solids. In van der Waals materials, this control can be achieved by modifying the stacking order through rotation and translation between the layers. Here, we observed stacking-dependent interlayer magnetism in the two-dimensional (2D) magnetic semiconductor chromium tribromide (CrBr3), which was enabled by the successful growth of its monolayer and bilayer through molecular beam epitaxy. Using in situ spin-polarized scanning tunneling microscopy and spectroscopy, we directly correlate the atomic lattice structure with the observed magnetic order. Although the individual monolayer CrBr3 is ferromagnetic, the interlayer coupling in bilayer depends on the stacking order and can be either ferromagnetic or antiferromagnetic. Our observations pave the way for manipulating 2D magnetism with layer twist angle control.

Natural van der Waals heterostructural single crystals with both magnetic and topological properties

Abstract: 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 observed below 5 K. The obtained homogeneous heterostructure with atomically sharp interface and intrinsic magnetic properties will be an ideal platform for studying the quantum anomalous Hall effect, axion insulator states, and the topological magnetoelectric effect.

Giant nonreciprocal second-harmonic generation from antiferromagnetic bilayer CrI 3

Abstract: Layered antiferromagnetism is the spatial arrangement of ferromagnetic layers with antiferromagnetic interlayer coupling. The van der Waals magnet chromium triiodide (CrI3) has been shown to be a layered antiferromagnetic insulator in its few-layer form1, opening up opportunities for various functionalities2-7 in electronic and optical devices. Here we report an emergent nonreciprocal second-order nonlinear optical effect in bilayer CrI3. The observed second-harmonic generation (SHG; a nonlinear optical process that converts two photons of the same frequency into one photon of twice the fundamental frequency) is several orders of magnitude larger than known magnetization-induced SHG8-11 and comparable to the SHG of the best (in terms of nonlinear susceptibility) two-dimensional nonlinear optical materials studied so far12,13 (for example, molybdenum disulfide). We show that although the parent lattice of bilayer CrI3 is centrosymmetric, and thus does not contribute to the SHG signal, the observed giant nonreciprocal SHG originates only from the layered antiferromagnetic order, which breaks both the spatial-inversion symmetry and the time-reversal symmetry. Furthermore, polarization-resolved measurements reveal underlying C2h crystallographic symmetry-and thus monoclinic stacking order-in bilayer CrI3, providing key structural information for the microscopic origin of layered antiferromagnetism14-18. Our results indicate that SHG is a highly sensitive probe of subtle magnetic orders and open up possibilities for the use of two-dimensional magnets in nonlinear and nonreciprocal optical devices.

Giant enhancement of interlayer exchange in an ultrathin 2D magnet

Abstract: Following the recent isolation of monolayer CrI3, there has been a surge of new two-dimensional van der Waals magnetic materials, whose incorporation in van der Waals heterostructures offers a new platform for spintronics, proximity magnetism, and quantum spin liquids. A primary question in this burgeoning field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies on CrI3 have shown a different magnetic ground state for ultrathin exfoliated films but the origin is not yet understood. Here, we use electron tunneling through few-layer crystals of the layered antiferromagnetic insulator CrCl3 to probe its magnetic order, finding a ten-fold enhancement in the interlayer exchange compared to bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveal that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low temperature stacking order and, we hypothesize, increased interlayer exchange. Our study provides new insight into the connection between stacking order and interlayer interactions in novel two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets, such as RuCl3.

Defect induced, layer-modulated magnetism in ultrathin metallic PtSe 2

Abstract: Defects are ubiquitous in solids and often introduce new properties that are absent in pristine materials. One of the opportunities offered by these crystal imperfections is an extrinsically induced long-range magnetic ordering1, a long-time subject of theoretical investigations1–3. Intrinsic, two-dimensional (2D) magnetic materials4–7 are attracting increasing attention for their unique properties, which include layer-dependent magnetism4 and electric field modulation6. Yet, to induce magnetism into otherwise non-magnetic 2D materials remains a challenge. Here we investigate magneto-transport properties of ultrathin PtSe2 crystals and demonstrate an unexpected magnetism. Our electrical measurements show the existence of either ferromagnetic or antiferromagnetic ground-state orderings that depends on the number of layers in this ultrathin material. The change in the device resistance on the application of a ~25 mT magnetic field is as high as 400 Ω with a magnetoresistance value of 5%. Our first-principles calculations suggest that surface magnetism induced by the presence of Pt vacancies and the Ruderman–Kittel–Kasuya–Yosida (RKKY) exchange couplings across ultrathin films of PtSe2 are responsible for the observed layer-dependent magnetism. Given the existence of such unavoidable growth-related vacancies in 2D materials8,9, these findings can expand the range of 2D ferromagnets into materials that would otherwise be overlooked. Magneto-transport measurements on thin metallic crystals of the transition metal dichalcogenide PtSe2 show signatures of ferro- and antiferromagnetic order depending on the number of layers and first-principles calculations suggest Pt vacancies at the surface as a plausible cause.

Field-tunable quantum disordered ground state in the triangular-lattice antiferromagnet NaYbO 2

Abstract: Antiferromagnetically coupled S = 1/2 spins on an isotropic triangular lattice are the paradigm of frustrated quantum magnetism, but structurally ideal realizations are rare. Here, we investigate NaYbO2, which hosts an ideal triangular lattice of effective Jeff = 1/2 moments with no inherent site disorder. No signatures of conventional magnetic order appear down to 50 mK, strongly suggesting a quantum spin liquid ground state. We observe a two-peak specific heat and a nearly quadratic temperature dependence, in agreement with expectations for a two-dimensional Dirac spin liquid. Application of a magnetic field strongly perturbs the quantum disordered ground state and induces a clear transition into a collinear ordered state, consistent with a long-predicted up–up–down structure for a triangular-lattice XXZ Hamiltonian driven by quantum fluctuations. The observation of spin liquid signatures in zero field and quantum-induced ordering in intermediate fields in the same compound demonstrates an intrinsically quantum disordered ground state. We conclude that NaYbO2 is a model, versatile platform for exploring spin liquid physics with full tunability of field and temperature. At zero magnetic field, the triangular-lattice antiferromagnet NaYbO2 shows the absence of long-range magnetic order down to 50 mK, consistent with quantum spin liquid behaviour. An external field renders the system a collinear ordered phase.

Mechanism of Néel Order Switching in Antiferromagnetic Thin Films Revealed by Magnetotransport and Direct Imaging.

Abstract: We probe the current-induced magnetic switching of insulating antiferromagnet-heavy-metal systems, by electrical spin Hall magnetoresistance measurements and direct imaging, identifying a reversal occurring by domain wall (DW) motion. We observe switching of more than one-third of the antiferromagnetic domains by the application of current pulses. Our data reveal two different magnetic switching mechanisms leading together to an efficient switching, namely, the spin-current induced effective magnetic anisotropy variation and the action of the spin torque on the DWs.

Interface-driven chiral magnetism and current-driven domain walls in insulating magnetic garnets

Abstract: Magnetic oxides exhibit rich fundamental physics1–4 and technologically desirable properties for spin-based memory, logic and signal transmission5–7. Recently, spin–orbit-induced spin transport phenomena have been realized in insulating magnetic oxides by using proximate heavy metal layers such as platinum8–10. In their metallic ferromagnet counterparts, such interfaces also give rise to a Dzyaloshinskii–Moriya interaction11–13 that can stabilize homochiral domain walls and skyrmions with efficient current-driven dynamics. However, chiral magnetism in centrosymmetric oxides has not yet been observed. Here we discover chiral magnetism that allows for pure spin-current-driven domain wall motion in the most ubiquitous class of magnetic oxides, ferrimagnetic iron garnets. We show that epitaxial rare-earth iron garnet films with perpendicular magnetic anisotropy exhibit homochiral Neel domain walls that can be propelled faster than 800 m s−1 by spin current from an adjacent platinum layer. We find that, despite the relatively small interfacial Dzyaloshinskii–Moriya interaction, very high velocities can be attained due to the antiferromagnetic spin dynamics associated with ferrimagnetic order. Spin currents from an adjacent Pt layer can drive homochiral Neel domain walls in centrosymmetric rare-earth iron garnet films at more than 800 m s–1, taking advantage of the antiferromagnetic spin dynamics of the ferrimagnetic oxide.

Voltage Control of a van der Waals Spin-Filter Magnetic Tunnel Junction

Abstract: 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 antialigned 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 can be switched reversibly between bistable magnetic states with the same net magnetization but drastically different resistance (by a factor of 10 or more). In addition, without switching the state, the TMR can be continuously modulated between 17,000% and 57,000%, due to the combination of spin-dependent tunnel barrier with changing carrier distributions in the graphene contacts. Our work demonstrates new kinds of ma...

Evidence of Spin Frustration in a Vanadium Diselenide Monolayer Magnet.

Abstract: Monolayer VSe2 , featuring both charge density wave and magnetism phenomena, represents a unique van der Waals magnet in the family of metallic 2D transition-metal dichalcogenides (2D-TMDs). Herein, by means of in situ microscopy and spectroscopic techniques, including scanning tunneling microscopy/spectroscopy, synchrotron X-ray and angle-resolved photoemission, and X-ray absorption, direct spectroscopic signatures are established, that identify the metallic 1T-phase and vanadium 3d1 electronic configuration in monolayer VSe2 grown on graphite by molecular-beam epitaxy. Element-specific X-ray magnetic circular dichroism, complemented with magnetic susceptibility measurements, further reveals monolayer VSe2 as a frustrated magnet, with its spins exhibiting subtle correlations, albeit in the absence of a long-range magnetic order down to 2 K and up to a 7 T magnetic field. This observation is attributed to the relative stability of the ferromagnetic and antiferromagnetic ground states, arising from its atomic-scale structural features, such as rotational disorders and edges. The results of this study extend the current understanding of metallic 2D-TMDs in the search for exotic low-dimensional quantum phenomena, and stimulate further theoretical and experimental studies on van der Waals monolayer magnets.

Manipulating exchange bias by spin–orbit torque

Abstract: Exchange bias, a shift in the hysteresis loop of a ferromagnet arising from interfacial exchange coupling between adjacent ferromagnetic and antiferromagnetic layers, is an integral part of spintronic devices. Here, we show that spin–orbit torque generated from spin current, a promising approach to switch the ferromagnetic magnetization of next-generation magnetic random access memory, can also be used to manipulate the exchange bias. Applying current pulses to a Pt/Co/IrMn trilayer causes concurrent switching of ferromagnetic magnetization and exchange bias, but with different underlying mechanisms. This implies that the ferromagnetic magnetization and exchange bias can be manipulated independently. Our work demonstrates that spin–orbit torque in ferromagnet/antiferromagnet heterostructures facilitates independent manipulations of distinct magnetic properties, motivating innovative designs for future spintronics devices. Spin–orbit torque is used to control the magnetic exchange bias in a Pt/Co/IrMn trilayer.

Suppression of magnetic ordering in XXZ-type antiferromagnetic monolayer NiPS3

Abstract: How a certain ground state of complex physical systems emerges, especially in two-dimensional materials, is a fundamental question in condensed-matter physics. A particularly interesting case is systems belonging to the class of XY Hamiltonian where the magnetic order parameter of conventional nature is unstable in two-dimensional materials leading to a Berezinskii-Kosterlitz-Thouless transition. Here, we report how the XXZ-type antiferromagnetic order of a magnetic van der Waals material, NiPS3, behaves upon reducing the thickness and ultimately becomes unstable in the monolayer limit. Our experimental data are consistent with the findings based on renormalization group theory that at low temperatures a two-dimensional XXZ system behaves like a two-dimensional XY one, which cannot have a long-range order at finite temperatures. This work provides experimental examination of the XY magnetism in the atomically thin limit and opens new opportunities of exploiting these fundamental theorems of magnetism using magnetic van der Waals materials.

Antiferromagnetic ordering in van der Waals 2D magnetic material MnPS 3 probed by Raman spectroscopy

Abstract: Magnetic ordering in the two-dimensional limit has been one of the most important issues in condensed matter physics for the past several decades. The recent discovery of new magnetic van der Waals materials heralds a much-needed easy route for the studies of two-dimensional magnetism: the thickness dependence of the magnetic ordering has been examined by using Ising- and XXZ-type magnetic van der Waals materials. Here, we investigated the magnetic ordering of MnPS3, a two-dimensional antiferromagnetic material of Heisenberg-type, by Raman spectroscopy from bulk all the way down to bilayer. The phonon modes that involve the vibrations of Mn ions exhibit characteristic changes as the temperature gets lowered through the Neel temperature. In bulk MnPS3, the Raman peak at ~155 cm-1 becomes considerably broadened near the Neel temperature and upon further cooling is subsequently red-shifted. The measured peak positions and polarization dependences of the Raman spectra are in excellent agreement with our first-principles calculations. In few-layer MnPS3, the peak at ~155 cm-1 exhibits the characteristic red-shift at low temperatures down to the bilayer, indicating that the magnetic ordering is surprisingly stable at such a thin limit. Our work sheds light on the hitherto unexplored magnetic ordering in the Heisenberg-type antiferromagnetic systems in the atomic-layer limit.

Natural van der Waals heterostructural single crystals with both magnetic and topological properties

Abstract: 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 observed below 5 K. The obtained homogeneous heterostructure with atomically sharp interface and intrinsic magnetic properties will be an ideal platform for studying the quantum anomalous Hall effect, axion insulator states, and the topological magnetoelectric effect.

Enhancement of interlayer exchange in an ultrathin two-dimensional magnet

Abstract: Following the recent isolation of monolayer CrI3 (ref. 1), many more two-dimensional van der Waals magnetic materials have been isolated2–12. Their incorporation in van der Waals heterostructures offers a new platform for spintronics5–9, proximity magnetism13 and quantum spin liquids14. A primary question in this field is how exfoliating crystals to the few-layer limit influences their magnetism. Studies of CrI3 have shown a different magnetic ground state for ultrathin exfoliated films1,5,6 compared with the bulk, but the origin is not yet understood. Here, we use electron tunnelling through few-layer crystals of the layered antiferromagnetic insulator CrCl3 to probe its magnetic order and find a tenfold enhancement of the interlayer exchange compared with bulk crystals. Moreover, temperature- and polarization-dependent Raman spectroscopy reveals that the crystallographic phase transition of bulk crystals does not occur in exfoliated films. This results in a different low-temperature stacking order and, we hypothesize, increased interlayer exchange. Our study provides insight into the connection between stacking order and interlayer interactions in two-dimensional magnets, which may be relevant for correlating stacking faults and mechanical deformations with the magnetic ground states of other more exotic layered magnets such as RuCl3 (ref. 14). Few-layer magnetic materials sometimes show a different form of magnetism from their thicker equivalents. The authors contend that the mechanism is changes in the stacking order in the thin limit that modify the interlayer exchange interaction.