2D Magnetism Research Articles

Substantially Enhanced Spin Polarization in Epitaxial CrTe2 Quantum Films.

2D van der Waals (vdW) magnets, which extend to the monolayer (ML) limit, are rapidly gaining prominence in logic applications for low-power electronics. To improve the performance of spintronic devices, such as vdW magnetic tunnel junctions, a large effective spin polarization of valence electrons is highly desired. Despite its considerable significance, direct probe of spin polarization in these 2D magnets has not been extensively explored. Here, using 2D vdW ferromagnet of CrTe2 as a prototype, the spin degrees of freedom in the thin films are directly probed using Mott polarimetry. The electronic band of 50 ML CrTe2 thin film, spanning the Brillouin zone, exhibits pronounced spin-splitting with polarization peaking at 7.9% along the out-of-plane direction. Surprisingly, atomic-layer-dependent spin-resolved measurements show a significantly enhanced spin polarization in a 3 ML CrTe2 film, achieving 23.4% polarization even in the absence of an external magnetic field. The demonstrated correlation between spin polarization and film thickness highlights the pivotal influence of perpendicular magnetic anisotropy, interlayer interactions, and itinerant behavior on these properties, as corroborated by theoretical analysis. This groundbreaking experimental verification of intrinsic effective spin polarization in CrTe2 ultrathin films marks a significant advance in establishing 2D ferromagnetic atomic layers as a promising platform for innovative vdW-based spintronic devices.

Recent Progress in Two-Dimensional Magnetic Materials.

The giant magnetoresistance effect in two-dimensional (2D) magnetic materials has sparked substantial interest in various fields; including sensing; data storage; electronics; and spintronics. Their unique 2D layered structures allow for the manifestation of distinctive physical properties and precise performance regulation under different conditions. In this review, we present an overview of this rapidly developing research area. Firstly, these 2D magnetic materials are catalogued according to magnetic coupling types. Then, several vital effects in 2D magnets are highlighted together with theoretical investigation, such as magnetic circular dichroism, magneto-optical Kerr effect, and anomalous Hall effect. After that, we forecast the potential applications of 2D magnetic materials for spintronic devices. Lastly, research advances in the attracting magnons, skyrmions and other spin textures in 2D magnets are discussed.

Single-Step Synthesis of An Ideal Chain Antiferromagnet [H2(4,4'-bipyridyl)](H3O)2Fe2F10 with Spin S=5/2.

One-dimensional (1D) magnets are of great interest owing to their intriguing quantum phenomena and potential application in quantum computing. We successfully synthesized an ideal antiferromagnetic spin S=5/2 chain compound [H2(4,4'-bpy)](H3O)2Fe2F10 (4,4'-bpy=4,4'-bipyridyl) 1, using a single-step low-temperature hydrothermal method under conditions that favors the protonation of the bulky bidentate ligand 4,4'-bpy. Compound 1 consists of well-separated (Fe3+-F-)∞ chains with a large Fe-F-Fe angle of 174.8°. Both magnetic susceptibility and specific heat measurements show that 1 does not undergo a magnetic long-range ordering down to 0.5 K, despite the strong Fe-F-Fe intrachain spin exchange J with J/kB=-16.2(1) K. This indicates a negligibly weak interchain spin exchange J'. The J'/J value estimated for 1 is extremely small (<2.8×10-6), smaller than those reported for all other S=5/2 chain magnets. Our hydrothermal synthesis incorporates both [H2(4,4'-bpy)]2+ and (H3O)+ cations into the crystal lattice with numerous hydrogen bonds, hence effectively separating the (Fe3+-F-)∞ spin chains. This single-step hydrothermal synthesis under conditions favoring the protonation of bulky bidentate ligands offers an effective synthetic strategy to prepare well-separated 1D spin chain systems of magnetic ions with various spin values.

Single‐Step Synthesis of An Ideal Chain Antiferromagnet [H2(4,4′‐bipyridyl)](H3O)2Fe2F10 with Spin S=5/2

AbstractOne‐dimensional (1D) magnets are of great interest owing to their intriguing quantum phenomena and potential application in quantum computing. We successfully synthesized an ideal antiferromagnetic spin S=5/2 chain compound [H2(4,4′‐bpy)](H3O)2Fe2F10 (4,4′‐bpy=4,4′‐bipyridyl) 1, using a single‐step low‐temperature hydrothermal method under conditions that favors the protonation of the bulky bidentate ligand 4,4′‐bpy. Compound 1 consists of well‐separated (Fe3+−F−)∞ chains with a large Fe−F−Fe angle of 174.8°. Both magnetic susceptibility and specific heat measurements show that 1 does not undergo a magnetic long‐range ordering down to 0.5 K, despite the strong Fe−F−Fe intrachain spin exchange J with J/kB=−16.2(1) K. This indicates a negligibly weak interchain spin exchange J′. The J′/J value estimated for 1 is extremely small (&lt;2.8×10−6), smaller than those reported for all other S=5/2 chain magnets. Our hydrothermal synthesis incorporates both [H2(4,4′‐bpy)]2+ and (H3O)+ cations into the crystal lattice with numerous hydrogen bonds, hence effectively separating the (Fe3+−F−)∞ spin chains. This single‐step hydrothermal synthesis under conditions favoring the protonation of bulky bidentate ligands offers an effective synthetic strategy to prepare well‐separated 1D spin chain systems of magnetic ions with various spin values.

Large Magnetic Anisotropy in van der Waals Ferromagnet Fe3GaTe2 above Room Temperature.

Discoveries of above-room-temperature intrinsic ferromagnetism in two-dimensional (2D) van der Waals (vdW) materials offer a platform for studying fundamental 2D magnetism and spintronic devices, especially the recently discovered above-room-temperature 2D vdW Fe3GaTe2 (FGaT). However, the magnetic mechanism in FGaT remains elusive. Here, a detailed investigation using magnetic force microscopy on the thickness-dependent magnetic behavior of FGaT single crystals is reported. The Heisenberg exchange interaction constant (J) at room temperature is determined to be 1.32836 × 10-12 J/m. Our study combining angle-resolved photoemission spectroscopy and density functional theory suggests that the high Curie temperature in FGaT is attributed to the shift of the localized Fe d band toward the Fermi level as well as the enhanced magnetic exchange effect due to the strong itinerant ability of Fe. This work sheds light on the understanding of magnetism in FGaT and provides a promising platform to investigate the mechanisms of 2D magnetic materials.

Strained van der Waals Metallic Magnet for Photomagnetic Modulation and Spin Photodiode Application

AbstractAll‐optical magnetization reversal provides a low‐power approach for investigating spin state manipulation in 2D magnets. However, the ambient observation of photomagnetic coupling presents significant challenges due to the low Curie temperatures exhibited by most 2D magnets. Herein, a mixed‐dimensional heterostructure comprising a surface‐oxidized Fe3GeTe2 nanosheet with enhanced magnetic properties and individual semiconducting ZnO nanorod is proposed to explore proximity photomagnetic modulation and spin‐enhanced photodetection behaviors. The surface curvature of ZnO nanorod induces pronounced strains for Fe3GeTe2 nanosheet, leading to its anomalous Raman polarization and spin ordering at room temperature. Strain‐activated itinerant spin electrons are immobilized on the O‐2p orbitals of adjacent ZnO, thereby facilitating the optical demagnetization process in Fe3GeTe2 without aid of magnetic field. First‐principles calculations together with in situ characterization experiments further confirm that the primary charge transfer channel involves coupling between Fe3+ and oxygen vacancy defects anchored at heterointerfaces. The rapid establishment of magnetization by illumination in ZnO nanorod contributes to spin‐tunneling‐enhanced photocurrent, device response dynamics, polarization detection and ultraviolet imaging capability. These findings offer valuable insights to optimize the optoelectronic properties of conventional semiconductors and advance complex dimensional spin‐optoelectronic devices.

2D magnets filled with lithium.

2D magnets filled with lithium.

Coexistence of ferroelectricity and antiferroelectricity in 2D van der Waals multiferroic

Multiferroic materials have been intensively pursued to achieve the mutual control of electric and magnetic properties. The breakthrough progress in 2D magnets and ferroelectrics encourages the exploration of low-dimensional multiferroics, which holds the promise of understanding inscrutable magnetoelectric coupling and inventing advanced spintronic devices. However, confirming ferroelectricity with optical techniques is challenging in 2D materials, particularly in conjunction with antiferromagnetic orders in single- and few-layer multiferroics. Here, we report the discovery of 2D vdW multiferroic with out-of-plane ferroelectric polarization in trilayer NiI2 device, as revealed by scanning reflective magnetic circular dichroism microscopy and ferroelectric hysteresis loops. The evolution between ferroelectric and antiferroelectric phases has been unambiguously observed. Moreover, the magnetoelectric interaction is directly probed by magnetic control of the multiferroic domain switching. This work opens up opportunities for exploring multiferroic orders and multiferroic physics at the limit of single or few atomic layers, and for creating advanced magnetoelectronic devices.

Sub-THz High Spin Precession Frequency in van der Waals Ferromagnet Fe3GaTe2.

The 2D magnet Fe3GaTe2 has received considerable attention for its high Curie temperature (TC), robust intrinsic ferromagnetism, and significant perpendicular magnetic anisotropy (PMA). In this study, the dynamic magnetic properties of Fe3GaTe2 are systematically investigated using an all-optical pump-probe technique. We find that the spin precession frequency (f) is as high as 351.2 GHz at T = 10 K under a field of H = 70 kOe. However, it decreases to 242.8 GHz at 300 K, mainly due to the reduced effective PMA field (Hkeff). The Gilbert damping factor (α) is modest, which increases from 0.039 (10 K) to 0.075 (300 K) owing to the enhanced scattering rate. Interestingly, when Fe3GaTe2 is coupled with 2 nm of Co, the Hkeff, f, and α just decrease slightly, highlighting the dominant influence of Fe3GaTe2. These findings substantially deepen our understanding of Fe3GaTe2, promoting the development of spintronic devices based on advanced 2D magnetic materials.

Magnetism Measurements of Two-Dimensional van der Waals Antiferromagnet CrPS4 Using Dynamic Cantilever Magnetometry

Abstract Recent experimental and theoretical work has focused on two-dimensional van der Waals (2D vdW) magnets due to their potential applications in sensing and spintronics devises. In measurements of these emerging materials, conventional magnetometry often encounters challenges in characterizing the magnetic properties of small-sized vdW materials, especially for antiferromagnets with nearly compensated magnetic moments. Here, we investigate the magnetism of 2D antiferromagnet CrPS4 with a thickness of 8 nm by using dynamic cantilever magnetometry (DCM). Through a combination of DCM experiment and the calculation based on a Stoner–Wohlfarth-type model, we unravel the magnetization states in 2D CrPS4 antiferromagnet. In the case of H ∥ c, a two-stage phase transition is observed. For H ⊥ c, a hump in the effective magnetic restoring force is noted, which implies the presence of spin reorientation as temperature increases. These results demonstrate the benefits of DCM for studying magnetism of 2D magnets.

Controlling Ultrafast Magnetization Dynamics via Coherent Phonon Excitation in a Ferromagnet Monolayer.

Exploring ultrafast magnetization control in 2D magnets via laser pulses is established, yet the interplay between spin dynamics and the lattice remains underexplored. Utilizing real-time time-dependent density functional theory (rt-TDDFT) coupled with Ehrenfest dynamics and nonadiabatic molecular dynamics (NAMD) simulations, we systematically investigate the laser-induced spin-nuclei dynamics with pre-excited A1g and E2g coherent phonons in the 2D ferromagnet Fe3GeTe2 (FGT) monolayer. Selective pre-excitation of coherent phonons under ultrafast laser irradiation significantly alters the local spin moment of FGT, consequently inducing additional spin loss attributed to the nuclear motion-induced asymmetric interatomic charge transfer. Excited spin-resolved charge undergoes a bidirectional spin-flip between spin-down and spin-up states, characterized by a subtle change in the spin moment within approximately 100 fs, followed by unidirectional spin-flip, which will further contribute to the spin moment loss of FGT within tens of picoseconds. Our results shed light on the coupling of coherent phonons with magnetization dynamics in 2D limit.

Anomalous Raman Response in 2D Magnetic FeTe Under Uniaxial Strain: Tetragonal and Hexagonal Polymorphs.

2D Fe-chalcogenides emerge with rich structures, magnetisms, and superconductivities, which spark the growing research interests in the torturous transition mechanism and tunable properties for their potential applications in nanoelectronics. Uniaxial strain can produce a lattice distortion to study symmetry breaking induced exotic properties in 2D magnets. Herein, the anomalous Raman spectrum of 2D tetragonal (t-) and hexagonal (h-) FeTe is systematically investigated via uniaxial strain engineering strategy. It is found that both t- and h-FeTe keep the structural stability under different uniaxial tensile or compressive strain up to ± 0.4%. Intriguingly, the lattice vibrations along both in-plane and out-of-plane directions exceptionally harden (softened) under tensile (compressive) strain, distinguished from the behaviors of many conventional 2D systems. Further, the difference in thickness-dependent strain effect can be well explained by their structural discrepancy between two polymorphs of FeTe. These results can supply a unique platform to explore the vibrational properties of many novel 2D materials.

Prospect for detecting magnetism in two-dimensional perovskite oxides by electron magnetic circular dichroism

Two-dimensional (2D) magnets, especially strongly correlated 2D transition-metal perovskite oxides, have attracted significant attention due to their intriguing electromagnetic properties for potential applications in spintronic devices. Potentially electron magnetic circular dichroism (EMCD) under zone axis conditions can provide three-dimensional components of magnetic moments in 2D materials, but the collection efficiency and the signal-to-noise ratio for out-of-plane (OOP) components is limited due to the limited collection angle. Here we conducted a comprehensive computational simulation to optimize the experimental setting of EMCD for detecting the OOP components of magnetic moments in three beam conditions (3BCs) on 2D perovskite oxides La1-xSrxMnO3 (LSMO) in a TEM. The key parameters are sample thickness, accelerating voltage, Sr doping concentration, collection semi-angle and position, and sample orientation including systematic reflections excited and tilt angle. Our simulation results demonstrate that the relative dynamical diffraction coefficients of Mn OOP EMCD of LaMnO3 with a thickness ranging from 1 unit cell (uc) to 4 uc can be optimized in a 3BC with (110) systematic reflections excited and a relatively large collection semi-angle of 19 mrad at the relatively low accelerating voltage of 80 kV. In most cases, the relative dynamic diffraction coefficients for La1-xSrxMnO3 with the thickness ranging from 1 uc to 4 uc decrease with the increase of the Sr doping concentrations. The optimal tilt angle from a zone axis to a 3BC is 18° for the cases of the LSMO thickness of 2 uc, 3 uc and 4 uc, and 22° for the monolayer LSMO. Our work provides the theoretical simulation foundation for optimized EMCD experiments for measuring OOP components of magnetic moments in 2D transition-metal perovskite oxides.

Above-room-temperature intrinsic ferromagnetism in ultrathin van der Waals crystal Fe3+xGaTe2

Two-dimensional (2D) van der Waals (vdW) magnets are crucial for ultra-compact spintronics. However, so far, no vdW crystal has exhibited tunable above-room-temperature intrinsic ferromagnetism in the 2D ultrathin regime. Here, we report the tunable above-room-temperature intrinsic ferromagnetism in ultrathin vdW crystal Fe3+xGaTe2 (x = 0 and 0.3). By increasing the Fe content, the Curie temperature (TC) and room-temperature saturation magnetization of bulk Fe3+xGaTe2 crystals are enhanced from 354 to 376 K and 43.9 to 50.4 emu·g−1, respectively. Remarkably, the robust anomalous Hall effect in 3-nm Fe3.3GaTe2 indicates a record-high TC of 340 K and a large room-temperature perpendicular magnetic anisotropy energy of 6.6 × 105 J m−3, superior to other ultrathin vdW ferromagnets. First-principles calculations reveal the asymmetric density of states and an additional large spin exchange interaction in ultrathin Fe3+xGaTe2 responsible for robust intrinsic ferromagnetism and higher TC. This work opens a window for above-room-temperature ultrathin 2D magnets in vdW-integrated spintronics.

Controllable growth of large 1T-NbTe2 nanosheets on mica by chemical vapor deposition and its magnetic properties

Two-dimensional (2D) magnetic materials have recently attracted broad attention for their potential technological applications. Here, we report controllable growth of NbTe2 nanosheets on mica substrate by atmospheric chemical vapor deposition. Different from the SiO2/Si substrates, dangling bonds on the surface of the mica are absent, which induces low nucleation density and higher lateral growth rate. As a result, the lateral size of NbTe2 nanosheets on mica substrates can be significantly larger than those on SiO2/Si substrates. Large single crystal NbTe2 nanosheets with a lateral size of up to 151 µm were fabricated on a mica. High-resolution transmission electron microscope image, XRD patterns and Raman spectra reveal the NbTe2 nanosheets adopt the single crystal with 1T phase. Furthermore, the NbTe2 nanosheets on mica demonstrate ferromagnetic properties with a Curie temperature of up to 162 K. Our work paves the way for the atmospheric chemical vapor deposition growth and applications of many more 2D magnets.

Unveiling the spin evolution in van der Waals antiferromagnets via magneto-exciton effects

Among the fascinating phenomena observed in two-dimensional (2D) magnets, the magneto-exciton effect stands out as a pivotal link between optics and magnetism. Although the excitonic effect has been revealed and exhibits a considerable correlation with the spin structures in certain 2D magnets, the underlying mechanism of the magneto-exciton effect remains underexplored, especially under high magnetic fields. Here we perform a systematic investigation of the spin-exciton coupling in 2D antiferromagnetic NiPS3 under high magnetic fields. When an in-plane magnetic field is applied, the exceptional sharp excitonic emission at ~1.4756 eV exhibits a Zeeman-like splitting with g ≈ 2.0, experimentally identifying the exciton as an excitation of dominant triplet-singlet character. By examining the polarization of excitonic emission and simulating the spin evolution, we further verify the correlation between excitonic emission and Néel vector in NiPS3. Our work elucidates the mechanism behind the spin-exciton coupling in NiPS3 and establishes a strategy for optically probing the spin evolutions in 2D magnets.

Epitaxial growth of quasi-2D van der Waals ferromagnets on crystalline substrates

Intrinsic magnetism in van der Waals materials has instigated interest in exploring magnetism in the 2D limit for potential applications in spintronics and also in understanding novel control of 2D magnetism via variation of layer thickness, gate tunability and magnetoelectric effects. The chromium telluride (CrxTey) family is an interesting subsection of ferromagnetic materials with highTCvalues, also presenting diverse stoichiometry arising from self-intercalation of Cr. Apart from the layered CrTe2system, the other non-layered CrxTeycompounds also offer exceptional magnetic properties, and a novel growth technique to grow thin films of these non-layered compounds offers exciting possibilities for ultra-thin spin-based electronics and magnetic sensors. In this work, we discuss the role of crystalline substrates in chemical vapor deposition growth of non-layered 2D ferromagnets, where the crystal symmetry of the substrate as well as the misfit and strain are the key players governing the growth mechanism of ultra-thin Cr5Te8, a non-layered ferromagnet. The magnetic studies of the as-grown Cr5Te8reveal the signatures of co-existing soft and hard ferromagnetic phases, which makes this system an intriguing system to search for emergent topological phases, such as magnetic skyrmions.

Nanotube spin defects for omnidirectional magnetic field sensing

Optically addressable spin defects in three-dimensional (3D) crystals and two-dimensional (2D) van der Waals (vdW) materials are revolutionizing nanoscale quantum sensing. Spin defects in one-dimensional (1D) vdW nanotubes will provide unique opportunities due to their small sizes in two dimensions and absence of dangling bonds on side walls. However, optically detected magnetic resonance of localized spin defects in a nanotube has not been observed. Here, we report the observation of single spin color centers in boron nitride nanotubes (BNNTs) at room temperature. Our findings suggest that these BNNT spin defects possess a spin S = 1/2 ground state without an intrinsic quantization axis, leading to orientation-independent magnetic field sensing. We harness this unique feature to observe anisotropic magnetization of a 2D magnet in magnetic fields along orthogonal directions, a challenge for conventional spin S = 1 defects such as diamond nitrogen-vacancy centers. Additionally, we develop a method to deterministically transfer a BNNT onto a cantilever and use it to demonstrate scanning probe magnetometry. Further refinement of our approach will enable atomic scale quantum sensing of magnetic fields in any direction.

Interfacial engineering of orbital orientation for perpendicular magnetic anisotropy in Co-implanted CrI3 monolayer

Two-dimensional (2D) van der Waals (vdW) magnets are believed to be promising candidates for next-generation information storage, which requires both high Curie points (TC) and large perpendicular magnetic anisotropy (PMA). As one of the most well-known 2D magnets, CrI3 has large PMA but a relatively low TC. Recent theoretical works proposed that implanting metal atoms into the hollow sites of CrI3 could greatly boost TC. However, this process may have the unintended consequence of reducing the PMA and introducing in-plane magnetic anisotropy (IMA) instead. It is, therefore, highly required to implement an additional technique to enhance the PMA. In this work, we use the first-principles method to study the underlying mechanisms of the suppressed PMA (and induced IMA) in the Co-implanted CrI3 monolayer [denoted as Co-(CrI3)2] as an example. It is found that the Co-implantation-induced itinerant electrons cause the transition from PMA to IMA by tuning the orbital orientation of the states around the Fermi level, noting that an in-plane (or out-of-plane) electronic orbital leads to the out-of-plane (or in-plane) momentum that favors PMA (or IMA) due to the spin–orbit coupling. In order to restore the PMA, we predict that using the vdW substrate PtTe2 to construct a heterostructure with the Co-(CrI3)2 monolayer not only reduces the contributions of the interfacial out-of-plane orbitals but also generates additional intralayer in-plane orbitals, both supporting the PMA. Thus, this work provides alternative perspectives on enhancing PMA by interfacial engineering of orbital orientation, paving the way for the development of 2D strong magnets.

Hybrid spin-orbit exciton-magnon excitations in FePS3

FePS3 is a layered van der Waals (vdW) Ising antiferromagnet that has recently been studied in the context of true 2D magnetism and emerged as an ideal material platform for investigating strong spin-phonon coupling, and non-linear magneto-optical phenomena. In this work, we demonstrate an important unresolved role of spin-orbit coupling (SOC) in the ground state and excitations of this compound. Combining first-principles calculations with linear flavor wave theory (LFWT), we find strong mixing and spectral overlap of different spin-orbital single-ion states. Low-lying excitations form hybrid spin-orbit exciton/magnon modes. Complete parameterization of the low-energy model requires nearly half a million coupling constants. Despite this complexity, such a model can be inexpensively derived using local many-body-based approaches, which yield quantitative agreement with recent experiments. The results highlight the importance of SOC even in first-row transition metals and provide essential insight into the properties of 2D magnets with unquenched orbital moments.