2D Magnetism Research Articles

Aged‐Precursor‐Assisted Growth of Ferrimagnetic 2D Cr9Se13 with Anomalous Elasticity

Abstract2D magnetic materials with distinct mechanical properties are of great importance for flexible spintronics. However, synthesizing 2D magnets with atomic thickness is challenging and their mechanical properties remain largely unexplored. Here, the growth of a ferrimagnetic 2D Cr9Se13 with anomalous elasticity is reported by an aged‐precursor‐assisted method. The obtained 2D Cr9Se13 exhibits an out‐of‐plane ferrimagnetic order with a coercivity larger than those of conventional magnetic materials. Noteworthy, it presents decent breaking strength and a Young's modulus of 52 ± 8 GPa that is among the smallest of the 2D family. This exceptional elasticity is attributed to the unique internal voids in Cr9Se13, as evidenced by the formed edge dislocations under strain. This work not only offers a facile method to synthesize 2D magnets but also develops avenues for obtaining 2D materials with desired mechanical properties, paving the way for future flexible spintronics.

Ferromagnetic Order in 2D Layers of Transition Metal Dichlorides.

Magnetism in two dimensions is traditionally considered an exotic phase mediated by spin fluctuations, but far from collinearly ordered in the ground state. Recently, 2D magnetic states have been discovered in layered van der Waals compounds. Their robust and tunable magnetic state by material composition, combined with reduced dimensionality, foresee a strong potential as a key element in magnetic devices. Here, a class of 2D magnets based on metallic chlorides is presented. The magnetic order survives on top of a metallic substrate, even down to the monolayer limit, and can be switched from perpendicular to in-plane by substituting the metal ion from iron to nickel. Using functionalized STM tips as magnetic sensors, local exchange fields are identified, even in the absence of an external magnetic field. Since the compounds are processable by molecular beam epitaxy techniques, they provide a platform with large potential for incorporation into current devicetechnologies.

Imaging the Magnetic Anisotropy in Ultrathin Fe4GeTe2 with a Nitrogen-Vacancy Magnetometer.

Two-dimensional (2D) FenGeTe2, with n = 3, 4, and 5, has been realized in experiments, showing strong magnetic anisotropy with enhanced critical temperature (Tc). The understanding of its magnetic anisotropy is crucial for the exploration of more stable 2D magnets and its spintronic applications. Here, we report a quantitative reconstruction of the magnetization magnitude and its direction in ultrathin Fe4GeTe2 using nitrogen vacancy centers. Through imaging stray magnetic fields, we identified the spin-flop transition at approximately 80 K, resulting in a change of the easy axis from the out-of-plane direction to the in-plane direction. Moreover, by analyzing the thermally activated escape behavior of the magnetization near Tc in terms of the Ginzburg-Landau model, we observed the in-plane magnetic anisotropy effect and the formation capability of magnetic domains at ∼0.4 μm2 μT-1. Our findings contribute to the quantitative understanding of the magnetic anisotropy effect in a vast range of 2D van der Waals magnets.

Impact of Spin-Entropy on the Thermoelectric Properties of a 2D Magnet.

Heat-to-charge conversion efficiency of thermoelectric materials is closely linked to the entropy per charge carrier. Thus, magnetic materials are promising building blocks for highly efficient energy harvesters as their carrier entropy is boosted by a spin degree of freedom. In this work, we investigate how this spin-entropy impacts heat-to-charge conversion in the A-type antiferromagnet CrSBr. We perform simultaneous measurements of electrical conductance and thermocurrent while changing magnetic order using the temperature and magnetic field as tuning parameters. We find a strong enhancement of the thermoelectric power factor at around the Néel temperature. We further reveal that the power factor at low temperatures can be increased by up to 600% upon applying a magnetic field. Our results demonstrate that the thermoelectric properties of 2D magnets can be optimized by exploiting the sizable impact of spin-entropy and confirm thermoelectric measurements as a sensitive tool to investigate subtle magnetic phase transitions in low-dimensional magnets.

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.

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.

Temperature‐Induced Structural Evolution and Magnetism in Self‐Intercalated V1+xSe2 Nanoplates

Abstract2D van der Waals (vdW) magnets provide the ideal platform for studying magnetism at low dimensions, where the magnetic properties can be further tuned by intercalating magnetic species and manipulating their stoichiometry and local atomic configuration. However, achieving stoichiometric intercalated 2D magnets necessitates precise control of growth parameters to avoid local compositional variations, which fosters phase coexistence that significantly impacts magnetic properties. Here a comprehensive scanning transmission electron microscopy (STEM) examination of the structural evolution in chemical vapor deposition (CVD)‐grown self‐intercalated V1+xSe2 nanoplates is shown, exploring their response to annealing temperature variations and the subsequent influence on magnetic properties. By combining ex situ and in situ post‐growth annealing, the rearrangement of intercalants is directly observed at the interlayer and identify a structural phase transition of the nanodomains embedded in the VSe2 matrix from V3Se4 to a V5Se8 structure occurring at ≈250 °C. The interlayer reconstruction is manifested by a positive‐to‐negative cross‐over in the magnetoresistance and an upturn in resistivity at low temperatures. The results provide new ways for tailoring 2D vdW magnets through post‐growth thermal annealing.

Distinct skyrmion phases at room temperature in two-dimensional ferromagnet Fe3GaTe2

Distinct skyrmion phases at room temperature hosted by one material offer additional degree of freedom for the design of topology-based compact and energetically-efficient spintronic devices. The field has been extended to low-dimensional magnets with the discovery of magnetism in two-dimensional van der Waals magnets. However, creating multiple skyrmion phases in 2D magnets, especially above room temperature, remains a major challenge. Here, we report the experimental observation of mixed-type skyrmions, exhibiting both Bloch and hybrid characteristics, in a room-temperature ferromagnet Fe3GaTe2. Analysis of the magnetic intensities under varied imaging conditions coupled with complementary simulations reveal that spontaneous Bloch skyrmions exist as the magnetic ground state with the coexistence of hybrid stripes domain, on account of the interplay between the dipolar interaction and the Dzyaloshinskii-Moriya interaction. Moreover, hybrid skyrmions are created and their coexisting phases with Bloch skyrmions exhibit considerably high thermostability, enduring up to 328 K. The findings open perspectives for 2D spintronic devices incorporating distinct skyrmion phases at room temperature.

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.

Thickness‐Dependent Crystal Structure, Synthesis, and Magnetism of Thin Film Chromium Chalcogenides: A Review

AbstractIn the search for two‐dimensional (2D) magnets operating under ambient conditions, quasi‐2D non‐van der Waals (vdW) materials have attracted considerable research interest over the last five years. In addition to their high Curie temperature (TC), their superior air stability to that of vdW 2D magnets has made them potential candidates for future room‐temperature spintronics applications. Furthermore, recent progress in the thickness‐dependent crystal lattice and magnetic properties of non‐vdW Cr2X3 (X = S, Se, or Te) has brought them to areas that are once set aside for 2D vdW magnets in fundamental research and applications. Despite covalent bonding between magnetic layers, various bottom‐up synthesis methods produced thickness‐controlled flakes of Cr2X3. Moreover, layer‐dependent structural and magnetic properties are among the novel research directions in these materials. This review systematically summarizes recent studies on Cr2X3 crystal structure, their controllable synthesis, and their respective magnetic properties. A summary of some significant results on thickness‐controlled synthesis in Cr2X3 and thickness‐dependent magnetism in Cr2Te3 is presented. Additionally, experimental and theoretical reports are presented to explain interlayer magnetic interaction. The work reveals the interaction between synthesis, structure, and magnetism. Finally, future research directions of new Cr2X3‐based materials, rich magnetism in Cr2X3, and their potential application are discussed.

Janus tetragonal Mn2BN monolayer: A 2D polar half-metal with coexistent ferroelectricity and magnetism

The integration of ferroelectricity, ferromagnetism, and half-metallicity in two-dimensional (2D) materials is pivotal for advancing spintronic device technologies. However, the progress in identifying such materials is limited, and we here propose a compelling approach by constructing asymmetry structures (Janus) based on known 2D magnets, namely, the Janus tetragonal Mn2BN monolayer as a promising polar half-metal. The asymmetric arrangement of B and N atoms, coupled with comparable atomic sizes and evident electronegativity, ensures structural stability and inherent polarization, while the dominance of Mn atoms governs magnetism. The robust ferromagnetic order stems from a strong super-exchange interaction, evident in the significant hybridization between Mn d and B/N p orbitals. The Mn2BN monolayer exhibits a wide spin bandgap (1.09 eV), a substantial electric polarization (9.15 μC cm−2), and a sizable magnetic anisotropic energy (238 μeV/Mn) and maintains stable ferromagnetic order to ∼800 K. These properties position it as a promising candidate for next-generation multifunctional devices in spintronics.

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.

Inverse Magnetocaloric Effect in Altermagnetic 2D Non‐van der Waals FeX (X = S and Se) Semiconductors

AbstractThe concept of altermagnet (AM), which is neither ferromagnet nor antiferromagnet, has recently been proposed as compensated collinear magnet. Among 2D non‐van der Waals crystals, one of the thinnest altermagnets is identified and their interesting physical phenomenon at 2D limit is investigated. According to symmetry analysis and first‐principles calculations, 2D FeX (X = S, Se) sheets with one‐unit‐cell thickness are intrinsic altermagnetic semiconductors with observable magnitude of spin splitting (103−193 meV), high magnetic transition temperature (TAM = 400 and 190 K), large out‐of‐plane magnetic anisotropy energy (0.24 and 0.74 meV per atom) and considerable metal‐like anomalous Hall conductivity (143 and 249 Ω−1 cm−1). Moreover, the spin lattices of these 2D FeX ultrathin films are formed by parallel diamond‐like chains with spin frustrated interaction through spin exchange along the b direction. Consequently, an inverse magnetocaloric effect with positive ∆Sm values of 1.7–8.2 mJ kg−1 K−1 near TAM is observed. These results enrich the database of altermagnets and provide deep insights into the spin frustration effect in 2D magnets, which paves the avenue for the next‐generation spintronics.

Magneto‐Optical Interactions in Layered Magnets

AbstractThe rapidly emerging field of 2D magnetic materials has garnered significant attention due to its fascinating physical properties and wide‐ranging potential applications. This review highlights the importance of magneto‐optical interactions as a crucial tool for both studying and modulating 2D magnets. It offers a comprehensive survey of current research concerning magneto‐optical interactions in 2D magnetic materials, encompassing the magneto‐optical Kerr effect, reflection magnetic circular dichroism, second‐harmonic generation, photoluminescence, inelastic light scattering, and time‐resolved spectroscopy. This review discusses how these techniques provide insights into the properties of 2D magnets, enabling exploration of magnetic phase transitions, lattice alterations, spin dynamics, as well as their responses to external fields. Moreover, it emphasizes the modulation of magnetic properties by photo‐stimulation and offers a brief outlook on this swiftly developing field.

Room‐temperature tunable tunneling magnetoresistance in Fe3GaTe2/WSe2/Fe3GaTe2 van der Waals heterostructures

AbstractThe exceptional properties of two‐dimensional (2D) magnet materials present a novel approach to fabricate functional magnetic tunnel junctions (MTJ) by constructing full van der Waals (vdW) heterostructures with atomically sharp and clean interfaces. The exploration of vdW MTJ devices with high working temperature and adjustable functionalities holds great potential for advancing the application of 2D materials in magnetic sensing and data storage. Here, we report the observation of highly tunable room‐temperature tunneling magnetoresistance through electronic means in a full vdW Fe3GaTe2/WSe2/Fe3GaTe2 MTJ. The spin valve effect of the MTJ can be detected even with the current below 1 nA, both at low and room temperatures, yielding a tunneling magnetoresistance (TMR) of 340% at 2 K and 50% at 300 K, respectively. Importantly, the magnitude and sign of TMR can be modulated by a DC bias current, even at room temperature, a capability that was previously unrealized in full vdW MTJs. This tunable TMR arises from the contribution of energy‐dependent localized spin states in the metallic ferromagnet Fe3GaTe2 during tunnel transport when a finite electrical bias is applied. Our work offers a new perspective for designing and exploring room‐temperature tunable spintronic devices based on vdW magnet heterostructures.

2D Ferroic Materials for Nonvolatile Memory Applications.

The emerging nonvolatile memory technologies based on ferroic materials are promising for producing high-speed, low-power, and high-density memory in the field ofintegrated circuits. Long-range ferroic orders observed in 2D materials have triggered extensive research interest in 2D magnets, 2D ferroelectrics, 2D multiferroics, and their device applications. Devices based on 2D ferroic materials and heterostructures with an atomically smooth interface and ultrathin thickness have exhibited impressive properties and significant potential for developing advanced nonvolatile memory. In this context, a systematic review of emergent 2D ferroic materials is conducted here, emphasizing their recent research on nonvolatile memory applications, with a view to proposing brighter prospects for 2D magnetic materials, 2D ferroelectric materials, 2D multiferroic materials, and their relevant devices.

Strain-driven valley-dependent Berry phase effects and topological transitions in Janus SVGeN2 monolayer

The manipulation of valley-dependent properties in two-dimensional (2D) materials is intriguing for developing valleytronics. Using first-principles calculations, we explore valley-dependent properties of Janus SVGeN2 monolayer and reveal large and tunable valley polarization by tensile strain. The SVGeN2 monolayer possesses excellent stability. Furthermore, strain-driven topological magneto-valley phase transitions are predicted for this monolayer, leading to the valley quantum anomalous Hall (VQAH) phenomenon. The VQAH state, which is featured by the coexistence of complete valley polarization and topological phase, is confirmed by sign reversal of Berry curvature and the nontrivial band topology. The calculated magnetic anisotropy energy indicates that the Janus SVGeN2 monolayer possesses a ferromagnetic ground state and in-plane magnetization. Our investigation provides some physical insights into the strain-driven topological phase transition and manipulation of valley-dependent properties to realize giant valley polarization in the Janus 2D magnet.

Electric control of optically-induced magnetization dynamics in a van der Waals ferromagnetic semiconductor

Electric control of magnetization dynamics in two-dimensional (2D) magnetic materials is an essential step for the development of novel spintronic nanodevices. Electrostatic gating has been shown to greatly affect the static magnetic properties of some van der Waals magnets, but the control over their magnetization dynamics is still largely unexplored. Here we show that the optically-induced magnetization dynamics in the van der Waals ferromagnet Cr2Ge2Te6 can be effectively controlled by electrostatic gates, with a one order of magnitude change in the precession amplitude and over 10% change in the internal effective field. In contrast to the purely thermally-induced mechanisms previously reported for 2D magnets, we find that coherent opto-magnetic phenomena play a major role in the excitation of magnetization dynamics in Cr2Ge2Te6. Our work sets the first steps towards electric control over the magnetization dynamics in 2D ferromagnetic semiconductors, demonstrating their potential for applications in ultrafast opto-magnonic devices.

Electrostatic Gating of Spin Dynamics of a Quasi-2D Kagome Magnet.

Electrostatic gating has emerged as a powerful technique for tailoring the magnetic properties of two-dimensional (2D) magnets, offering exciting prospects including enhancement of magnetic anisotropy, boosting Curie temperature, and strengthening exchange coupling effects. Here, we focus on electrical control of the ferromagnetic resonance of the quasi-2D Kagome magnet Cu(1,3-bdc). By harnessing an electrostatic field through ionic liquid gating, significant shifts are observed in the ferromagnetic resonance field in both out-of-plane and in-plane measurements. Moreover, the effective magnetization and gyromagnetic ratios display voltage-dependent variations. A closer examination reveals that the voltage-induced changes can modulate magnetocrystalline anisotropy by several hundred gauss, while the impact on orbital magnetization remains relatively subtle. Density functional theory (DFT) calculations reveal varying d-orbital hybridizations at different voltages. This research unveils intricate physics within the Kagome lattice magnet and further underscores the potential of electrostatic manipulation in steering magnetism with promising implications for the development of spintronic devices.

Room-temperature sub-100 nm Néel-type skyrmions in non-stoichiometric van der Waals ferromagnet Fe3-xGaTe2 with ultrafast laser writability

Realizing room-temperature magnetic skyrmions in two-dimensional van der Waals ferromagnets offers unparalleled prospects for future spintronic applications. However, due to the intrinsic spin fluctuations that suppress atomic long-range magnetic order and the inherent inversion crystal symmetry that excludes the presence of the Dzyaloshinskii-Moriya interaction, achieving room-temperature skyrmions in 2D magnets remains a formidable challenge. In this study, we target room-temperature 2D magnet Fe3GaTe2 and unveil that the introduction of iron-deficient into this compound enables spatial inversion symmetry breaking, thus inducing a significant Dzyaloshinskii-Moriya interaction that brings about room-temperature Néel-type skyrmions with unprecedentedly small size. To further enhance the practical applications of this finding, we employ a homemade in-situ optical Lorentz transmission electron microscopy to demonstrate ultrafast writing of skyrmions in Fe3-xGaTe2 using a single femtosecond laser pulse. Our results manifest the Fe3-xGaTe2 as a promising building block for realizing skyrmion-based magneto-optical functionalities.