Two-dimensional Magnets Research Articles

Alternating spin splitting of electronic and magnon bands in two-dimensional altermagnetic materials

Abstract Unconventional antiferromagnetism dubbed as altermagnetism was firstly discovered in rutile structured magnets, which is featured by spin splitting even without the spin-orbit coupling effect. This interesting phenomenon has led to the discovery of more altermagnetic materials. In this work, we explore two-dimensional altermagnetic materials by studying two series of two-dimensional magnets, including MF4 with M covering all 3d and 4d transition metal elements, as well as TS2 with T = V, Cr, Mn, Fe. Through the magnetic symmetry operation of the RuF4 and MnS2, it was verified that breaking the time inversion is a necessary condition for spin splitting. Based on symmetry analysis and first-principles calculations, we found that the electronic bands and magnon dispersion experience alternating spin splitting along the same path. This work paves the way for exploring altermagnetism in two-dimensional materials.

Magnetic Structure-Dependent Ultrafast Spin Relaxation in Magnet CrI3: A Time-Domain ab Initio Study.

Two-dimensional magnet CrI3 is a promising candidate for spintronic devices. Using nonadiabatic molecular dynamics and noncollinear spin time-dependent density functional theory, we investigated hole spin relaxation in two-dimensional CrI3 and its dependence on magnetic configurations, impacted by spin-orbit and electron-phonon interactions. Driven by in-plane and out-of-plane iodine motions, the relaxation rates vary, extending from over half a picosecond in ferromagnetic systems to tens of femtoseconds in certain antiferromagnetic states due to significant spin fluctuations, associated with the nonadiabatic spin-flip in tuning to the adiabatic flip. Antiferromagnetic CrI3 with staggered layer magnetic order notably accelerates adiabatic spin-flip due to enhanced state degeneracy and additional phonon modes. Ferrimagnetic CrI3 shows a transitional behavior between ferromagnetic and antiferromagnetic types as the magnetic moment changes. These insights into the spin dynamics of CrI3 underscore its potential for rapid-response spintronic applications and advance our understanding of two-dimensional materials for spintronics.

Impact of dimensionality on the magnetocaloric effect in two-dimensional magnets

Magnetocaloric materials, which exploit reversible temperature changes induced by magnetic field variations, are promising for advancing energy-efficient cooling technologies. The potential integration of two-dimensional materials into magnetocaloric systems represents an emerging opportunity to enhance the magnetocaloric cooling efficiency. In this study, we use atomistic spin dynamics simulations based on first-principles parameters to systematically evaluate how magnetocaloric properties transition from three-dimensional (3D) to two-dimensional (2D) ferromagnetic materials. We find that 2D features such as reduced Curie temperature, sharper magnetic transition, and higher magnetic susceptibility are beneficial for magnetocaloric applications, while the relatively higher lattice heat capacity in 2D can compromise achievable adiabatic temperature changes. We further propose GdSi2 as a promising 2D magnetocaloric material. Our calculation predicts that GdSi2 exhibits an isothermal entropy change ΔSM of 22.5 J kg−1 K−1 and an adiabatic temperature change ΔTad of 6.2 K, near the hydrogen liquefaction temperature (TC≈25 K). Our analysis offers valuable theoretical insights into the magnetocaloric effect in 2D ferromagnets and demonstrates that 2D ferromagnets hold promise for cooling and thermal management applications in compact and miniaturized nanodevices.

Influence of Magnetic Sublattice Ordering on Skyrmion Bubble Stability in 2D Magnet Fe5GeTe2.

The realization of above room-temperature ferromagnetism in the two-dimensional (2D) magnet Fe5GeTe2 represents a major advance for the use of van der Waals (vdW) materials in practical spintronic applications. In particular, observations of magnetic skyrmions and related states within exfoliated flakes of this material provide a pathway to the fine-tuning of topological spin textures via 2D material heterostructure engineering. However, there are conflicting reports as to the nature of the magnetic structures in Fe5GeTe2. The matter is further complicated by the study of two types of Fe5GeTe2 crystals with markedly different structural and magnetic properties, distinguished by their specific fabrication procedure: whether they are slowly cooled or rapidly quenched from the growth temperature. In this work, we combine X-ray and electron microscopy to observe the formation of magnetic stripe domains, skyrmion-like type-I, and topologically trivial type-II bubbles, within exfoliated flakes of Fe5GeTe2. The results reveal the influence of the magnetic ordering of the Fe1 sublattice below 150 K, which dramatically alters the magnetocrystalline anisotropy and leads to a complex magnetic phase diagram and a sudden change of the stability of the magnetic textures. In addition, we highlight the significant differences in the magnetic structures intrinsic to slow-cooled and quenched Fe5GeTe2 flakes.

Enhanced magnetic transition temperature through ferromagnetic and antiferromagnetic interaction in cobalt-substituted Fe5GeTe2

Two-dimensional (2D) magnetism is an incredibly intriguing phenomenon in condensed matter physics. The exploration of 2D magnets holds great promise for various applications, even though they often exhibit low magnetic transition temperature. Among these materials, Fe5GeTe2 has emerged as a compelling candidate for room-temperature spintronics due to its intrinsic ferromagnetism and high Curie temperature. In this study, we investigate the impact of Co substitution at the Fe sites in Fe5GeTe2, which induces a transition of the magnetic ground state to the antiferromagnetic state when the substitution level exceeds 0.36. Additionally, we observe the coexistence of ferromagnetic (FM) and antiferromagnetic states in the magnetic transition region of (Fe1−xCox)5GeTe2 crystals. Notably, the interaction between the two magnetic phases results in Néel temperature (TN) up to 374 K, establishing a record among known van der Waals antiferromagnets. Our findings present a strategy for enhancing the magnetic temperature of 2D magnets, paving the way for potential advancements in spintronics applications.

Deep learning methods for Hamiltonian parameter estimation and magnetic domain image generation in twisted van der Waals magnets

The application of twist engineering in van der Waals magnets has opened new frontiers in the field of two-dimensional magnetism, yielding distinctive magnetic domain structures. Despite the introduction of numerous theoretical methods, limitations persist in terms of accuracy or efficiency due to the complex nature of the magnetic Hamiltonians pertinent to these systems. In this study, we introduce a deep-learning approach to tackle these challenges. Utilizing customized, fully connected networks, we develop two deep-neural-network kernels that facilitate efficient and reliable analysis of twisted van der Waals magnets. Our regression model is adept at estimating the magnetic Hamiltonian parameters of twisted bilayer CrI3 from its magnetic domain images generated through atomistic spin simulations. The ‘generative model’ excels in producing precise magnetic domain images from the provided magnetic parameters. The trained networks for these models undergo thorough validation, including statistical error analysis and assessment of robustness against noisy injections. These advancements not only extend the applicability of deep-learning methods to twisted van der Waals magnets but also streamline future investigations into these captivating yet poorly understood systems.

Anomalous Hall effect sensitive to magnetic monopoles and skyrmion helicity in spin–orbit coupled systems

Magnetic textures, such as skyrmions and domain walls, engender rich transport phenomena, including anomalous Hall effect and nonlinear response. In this work, we discuss an anomalous Hall effect proportional to the net magnetic monopole charge and dependent on the skyrmion helicity that occurs by a skew scattering in a noncentrosymmetric two-dimensional magnet. This mechanism, which arises from the spin–orbit interaction (SOI), gives rise to a finite anomalous Hall effect in a ferromagnetic domain wall whose spins rotate in the xy plane despite no out-of-plane magnetic moment. We show that the presence and absence of the monopole contribution is related to crystal symmetry, which gives a guideline for finding candidate materials beyond the Rashba model. The results demonstrate the rich features arising from the interplay of SOI and magnetic textures, and their potential for detecting various magnetic textures in micrometer devices.

All-optical control of skyrmion configuration in CrI monolayer.

The potential for manipulating characteristics of skyrmions in a CrI monolayer using circularly polarised light is explored. The effective skyrmion-light interaction is mediated by bright excitons whose magnetization is selectively influenced by the polarization of photons. The light-induced skyrmion dynamics is illustrated by the dependencies of the skyrmion size and the skyrmion lifetime on the intensity and polarization of the incident light pulse. Two-dimensional magnets hosting excitons thus represent a promising platform for the control of topological magnetic structures by light.

Tailoring coercive fields and the Curie temperature via proximity coupling in WSe2/Fe3GeTe2 van der Waals heterostructures

Hybrid structures consisting of two-dimensional (2D) magnets and semiconductors have exhibited extensive functionalities in spintronics and opto-spintronics. In this work, we have fabricated WSe2/Fe3GeTe2 van der Waals heterostructures and investigated proximity effects on 2D magnetism. Through reflective magnetic circular dichroism, we have observed a temperature-dependent modulation of magnetic order in the heterostructure. For temperatures above 40K , WSe2-covered Fe3GeTe2 exhibits a larger coercive field than that observed in bare Fe3GeTe2, accompanied by a noticeable enhancement of the Curie temperature by 21K . This strengthening suggests an increase in magnetic anisotropy in the interfacial Fe3GeTe2 layer, which can be attributed to the spin–orbit coupling (SOC) proximity effect induced by the adjacent WSe2 layers. However, at much lower temperatures ( T<20K ), a non-monotonic modification of the coercive field is observed, showing both reduction and enhancement, which depends on the thickness of the WSe2 and Fe3GeTe2 layers. Moreover, an unconventional two-step magnetization process emerges in the heterostructure, indicating the short-range nature of SOC proximity effects. Our findings on proximity coupling may shed light on the design of future spintronic and memory devices based on 2D magnetic heterostructures.

Spin disorder control of topological spin texture

Stabilization of topological spin textures in layered magnets has the potential to drive the development of advanced low-dimensional spintronics devices. However, achieving reliable and flexible manipulation of the topological spin textures beyond skyrmion in a two-dimensional magnet system remains challenging. Here, we demonstrate the introduction of magnetic iron atoms between the van der Waals gap of a layered magnet, Fe3GaTe2, to modify local anisotropic magnetic interactions. Consequently, we present direct observations of the order-disorder skyrmion lattices transition. In addition, non-trivial topological solitons, such as skyrmioniums and skyrmion bags, are realized at room temperature. Our work highlights the influence of random spin control of non-trivial topological spin textures.

Tunneling current-controlled spin states in few-layer van der Waals magnets.

Effective control of magnetic phases in two-dimensional magnets would constitute crucial progress in spintronics, holding great potential for future computing technologies. Here, we report a new approach of leveraging tunneling current as a tool for controlling spin states in CrI3. We reveal that a tunneling current can deterministically switch between spin-parallel and spin-antiparallel states in few-layer CrI3, depending on the polarity and amplitude of the current. We propose a mechanism involving nonequilibrium spin accumulation in the graphene electrodes in contact with the CrI3 layers. We further demonstrate tunneling current-tunable stochastic switching between multiple spin states of the CrI3 tunnel devices, which goes beyond conventional bi-stable stochastic magnetic tunnel junctions and has not been documented in two-dimensional magnets. Our findings not only address the existing knowledge gap concerning the influence of tunneling currents in controlling the magnetism in two-dimensional magnets, but also unlock possibilities for energy-efficient probabilistic and neuromorphic computing.

Monte Carlo Based Techniques for Quantum Magnets with Long-Range Interactions.

Long-range interactions are relevant for a large variety of quantum systems in quantum optics and condensed matter physics. In particular, the control of quantum-optical platforms promises to gain deep insights into quantum-critical properties induced by the long-range nature of interactions. From a theoretical perspective, long-range interactions are notoriously complicated to treat. Here, we give an overview of recent advancements to investigate quantum magnets with long-range interactions focusing on two techniques based on Monte Carlo integration. First, the method of perturbative continuous unitary transformations where classical Monte Carlo integration is applied within the embedding scheme of white graphs. This linked-cluster expansion allows extracting high-order series expansions of energies and observables in the thermodynamic limit. Second, stochastic series expansion quantum Monte Carlo integration enables calculations on large finite systems. Finite-size scaling can then be used to determine the physical properties of the infinite system. In recent years, both techniques have been applied successfully to one- and two-dimensional quantum magnets involving long-range Ising, XY, and Heisenberg interactions on various bipartite and non-bipartite lattices. Here, we summarise the obtained quantum-critical properties including critical exponents for all these systems in a coherent way. Further, we review how long-range interactions are used to study quantum phase transitions above the upper critical dimension and the scaling techniques to extract these quantum critical properties from the numerical calculations.

Giant and controllable nonlinear magneto-optical effects in two-dimensional magnets

The interplay of polarization and magnetism in materials with light can create rich nonlinear magneto-optical (NLMO) effects, and the recent discovery of two-dimensional (2D) van der Waals magnets provides remarkable control over NLMO effects due to their superb tunability. Here, based on first-principles calculations, we reported giant NLMO effects in CrI3-based 2D magnets, including a dramatic change of second-harmonics generation (SHG) polarization direction (90°) and intensity (on/off switch) under magnetization reversal and a 100% SHG circular dichroism effect. We further revealed that these effects could not only be used to design ultra-thin multifunctional optical devices but also to detect subtle magnetic orderings. Remarkably, we analytically derived conditions to achieve giant NLMO effects and proposed general strategies to realize them in 2D magnets. Our work not only uncovers a series of intriguing NLMO phenomena but also paves the way for both fundamental research and device applications of ultra-thin NLMO materials.

Alloying Driven Antiferromagnetic Skyrmions on NiPS3 Monolayer: A First-Principles Calculation.

Topological magnetic states are promising information carriers for ultrahigh-density and high-efficiency magnetic storage. Recent advances in two-dimensional (2D) magnets provide powerful platforms for stabilizing various nanometer-size topological spin textures within a wide range of magnetic field and temperature. However, non-centrosymmetric 2D magnets with broken inversion symmetry are scarce in nature, making direct observations of the chiral spin structure difficult, especially for antiferromagnetic (AFM) skyrmions. In this work, it is theoretically predicted that intrinsic AFM skyrmions can be easily triggered in XY-type honeycomb magnet NiPS3 monolayer by alloying of Cr atoms, due to the presence of a sizable Dzyaloshinskii-Moriya interaction. More interestingly, the diameter of the AFM skyrmions in Ni3/4Cr1/4PS3 decreases from 12 to 4.4nm as the external magnetic field increases and the skyrmion phases remain stable up to an external magnetic field of 4 T. These results highlight an effective strategy to generate and modulate the topological spin texture in 2D magnets by alloying with magnetic element.

Temperature-dependent anisotropy variation in quasi-two-dimensional ferromagnetic Cr5Te8

The quasi-two-dimensional ferromagnet Cr5Te8 is a promising material for spintronic devices due to its near-room-temperature Curie temperature (TC), strong magnetic anisotropy, and easily controllable properties. In this study, the anisotropic magnetization of trigonal (T-) Cr5Te8 single crystals is investigated. Our magnetization study reveals that a ferromagnetic transition occurs when the magnetic field is aligned parallel to the c-axis (H//c), while an antiferromagnetic transition appears for H//ab, with a strong perpendicular anisotropy in the ground state. However, electron spin resonance (ESR) spectroscopy indicates that the direction of the easy-axis changes from the c-axis to the ab-plane at TV∼ 190 K as the temperature increases. Furthermore, angle-dependent ESR spectra demonstrate a characteristic of two-dimensional magnetism in the bulk Cr5Te8 single crystal. It is suggested that the temperature-dependent variation in anisotropy is caused by changes in lattice structure through the tuning of the dominant direct-exchange between the intralayers and the super-exchange within the interlayers. The temperature- and field-dependent microwave responses of T-Cr5Te8 are advantageous for the application of this material as a microwave-based spintronic device.

Quantum Electrodynamics in 2+1 Dimensions as the Organizing Principle of a Triangular Lattice Antiferromagnet

Quantum electrodynamics in 2+1 dimensions (QED3) has been proposed as a critical field theory describing the low-energy effective theory of a putative algebraic Dirac spin liquid or of quantum phase transitions in two-dimensional frustrated magnets. We provide compelling evidence that the intricate spectrum of excitations of the elementary but strongly frustrated J1−J2 Heisenberg model on the triangular lattice is in one-to-one correspondence to a zoo of excitations from QED3, in the quantum spin liquid regime. This evidence includes a large manifold of explicitly constructed monopole and bilinear excitations of QED3, which is thus shown to serve as an organizing principle of phases of matter in triangular lattice antiferromagnets and their low-lying excitations. Moreover, we observe signatures of emergent valence-bond solid (VBS) correlations, which can be interpreted either as evidence of critical VBS fluctuations of an emergent Dirac spin liquid or as a transition from the 120° Néel order to a VBS whose quantum critical point is described by QED3. Our results are obtained by comparing ansatz wave functions from a parton construction to exact eigenstates obtained using large-scale exact diagonalization up to N=48 sites. Published by the American Physical Society 2024

Structural distortion and dynamical electron correlation driven enhanced ferromagnetism in Ni-doped two-dimensional Fe5GeTe2 beyond room temperature

Achieving beyond room-temperature ferromagnetism in two-dimensional (2D) magnets is immensely desirable for spintronic applications. Fe5GeTe2 is an exceptional van der Waals metallic ferromagnet due to its tunable physical properties and relatively higher Curie temperature ( TC ) than other 2D magnets. Using density functional theory combined with dynamical electron correlation and Monte Carlo simulations, we find the TC of (Fe 1−δ Ni δ)5 GeTe2 monolayer can increase up to ∼400 K at δ∼0.20 (δ: fractional occupation). Two specific Fe sublattices are identified to be the most energetically preferred sites to host Ni. Exchange interactions between particular Fe pairs play a dominating role in controlling TC , influenced by the dopant-induced structural distortions. Dynamical electron correlation induces site- and orbital-specific quasi-particle mass of Fe-d states with varying Ni concentrations. This work provides fundamental insights into 2D magnetism as an interplay of structural and electronic aspects and would guide to tailoring exciting magnetic phenomena in similar systems.

Monolayer Fe3GaX2 (X = I, Br, Sb): High-Temperature Two-Dimensional Magnets and a Novel Partially Ordered Spin State

Monolayer Fe₃GaX₂ (X = I, Br, Sb): High-Temperature Two-Dimensional Magnets and a Novel Partially Ordered Spin State

Evidence of Ferromagnetism and Ultrafast Dynamics of Demagnetization in an Epitaxial FeCl2 Monolayer.

The development of two-dimensional (2D) magnetism is driven not only by the interest of low-dimensional physics but also by potential applications in high-density miniaturized spintronic devices. However, 2D materials possessing a ferromagnetic order with a relatively high Curie temperature (Tc) are rare. In this paper, the evidence of ferromagnetism in monolayer FeCl2 on Au(111) surfaces, as well as the interlayer antiferromagnetic coupling of bilayer FeCl2, is characterized by using spin-polarized scanning tunneling microscopy. A Curie temperature (Tc) of ∼147 K is revealed for monolayer FeCl2, based on our static magneto-optical Kerr effect measurements. Furthermore, temperature-dependent magnetization dynamics is investigated by the time-resolved magneto-optical Kerr effect. A transition from one- to two-step demagnetization occurs as the lattice temperature approaches Tc, which supports the Elliott-Yafet spin relaxation mechanism. The findings contribute to a deeper understanding of the underlying mechanisms governing ultrafast magnetization in 2D ferromagnetic materials.

Topological Kerr effects in two-dimensional magnets with broken inversion symmetry

Topological Kerr effects in two-dimensional magnets with broken inversion symmetry