2D Ferromagnets Research Articles

Strong variation of spin-orbit torques with relative spin relaxation rates in ferrimagnets

Spin-orbit torques (SOTs) have been widely understood as an interfacial transfer of spin that is independent of the bulk properties of the magnetic layer. Here, we report that SOTs acting on ferrimagnetic FexTb1-x layers decrease and vanish upon approaching the magnetic compensation point because the rate of spin transfer to the magnetization becomes much slower than the rate of spin relaxation into the crystal lattice due to spin-orbit scattering. These results indicate that the relative rates of competing spin relaxation processes within magnetic layers play a critical role in determining the strength of SOTs, which provides a unified understanding for the diverse and even seemingly puzzling SOT phenomena in ferromagnetic and compensated systems. Our work indicates that spin-orbit scattering within the magnet should be minimized for efficient SOT devices. We also find that the interfacial spin-mixing conductance of interfaces of ferrimagnetic alloys (such as FexTb1-x) is as large as that of 3d ferromagnets and insensitive to the degree of magnetic compensation.

Tuning the Magnetic Anisotropy of Co–N‐Doped Graphene

Large magnetic anisotropy energy and out‐of‐plane easy magnetization direction are beneficial for the application of 2D ferromagnetism. Although the robust room‐temperature ferromagnetism is reported in Co–N‐doped graphene [Nat. Commun. 2021, 12, 1854], its magnetic anisotropy and easy axis of magnetization are still unclear. Herein, the magnetic anisotropy of CoN4–graphene and CoN3–graphene is systematically studied. The CoN4–graphene has an in‐plane easy magnetization direction, while the easy magnetization direction of CoN3–graphene is out‐of‐plane. The magnetic anisotropy energy can be tuned by injecting charge or applying strain. Especially, for CoN3–graphene, both charge injection and tensile strain can tune the easy magnetization direction from out‐of‐plane to in‐plane. The tunable magnetic anisotropy may promote the application of Co–N‐doped graphene in spintronic devices.

Higher-order nonlinear anomalous Hall effects induced by Berry curvature multipoles

In recent years, it has been shown that Berry curvature monopoles and dipoles play essential roles in the anomalous Hall and the nonlinear Hall effects, respectively. In this work, we demonstrate that Berry curvature multipoles (the higher moments of Berry curvatures at the Fermi energy) can induce higher-order nonlinear anomalous Hall (NLAH) effects. Specifically, an AC Hall voltage perpendicular to the current direction emerges, where the frequency is an integer multiple of the frequency of the applied current. Importantly, by analyzing the symmetry properties of all the 3D and 2D magnetic point groups, we note that the quadrupole, hexapole, and even higher Berry curvature moments can cause the leading-order frequency multiplication in certain materials. To provide concrete examples, we point out that the third-order NLAH voltage can be the leading-order Hall response in certain antiferromagnets due to Berry curvature quadrupoles, and the fourth-order NLAH voltage can be the leading response in the surface states of topological insulators induced by Berry curvature hexapoles. Our results are established by symmetry analysis, effective Hamiltonian, and first-principles calculations. Other materials which support the higher-order NLAH effect are further proposed, including 2D antiferromagnets and ferromagnets, Weyl semimetals, and twisted bilayer graphene near the quantum anomalous Hall phase.

Strongly Correlated Exciton-Magnetization System for Optical Spin Pumping in CrBr3 and CrI3 .

Ferromagnetism in van der Waals systems, preserved down to a monolayer limit, attracted attention to a class of materials with general composition CrX3 (X=I, Br, and Cl), which are treated now as canonical 2D ferromagnets. Their diverse magnetic properties, such as different easy axes or varying and controllable character of in-plane or interlayer ferromagnetic coupling, make them promising candidates for spintronic, photonic, optoelectronic, and other applications. Still, significantly different magneto-optical properties between the three materials have been presenting a challenging puzzle for researchers over the last few years. Herewith, it is demonstrated that despite similar structural and magnetic configurations, the coupling between excitons and magnetization is qualitatively different in CrBr3 and CrI3 films. Through a combination of the optical spin pumping experiments with the state-of-the-art theory describing bound excitonic states in the presence of magnetization, weconcluded that the hole-magnetization coupling has the opposite sign in CrBr3 and CrI3 and also between the ground and excited exciton state. Consequently, efficient spin pumping capabilities are demonstrated in CrBr3 driven by magnetization via spin-dependent absorption, and the different origins of the magnetic hysteresis in CrBr3 and CrI3 are unraveled.

Even-Odd-Layer-Dependent Ferromagnetism in 2D Non-van-der-Waals CrCuSe2.

Van der Waals (vdW) layered materials with strong magnetocrystalline anisotropy have attracted significant interest as the long-range magnetic order in these systems can survive even when their thicknesses is reduced to the 2D limit. Even though the interlayer coupling between the neighboring magnetic layers is very weak, it has a determining effect on the magnetism of these atomic-thickness materials. Herein, a new 2D ferromagnetic material, namely, non-vdW CuCrSe2 nanosheets with even-odd-layer-dependent ferromagnetism when laminated from an antiferromagnetic bulk is reported. Monolayer and even-layer CuCrSe2 exhibit the anomalous Hall effect and a significantly enhanced magnetic ordering temperature of more than 125 K. In contrast, the linear Hall effect exists in the odd-layer samples. Theoretical calculations indicate that the layer-dependent magnetic coupling is attributable to the orbital shift of the Cr atoms in the CrSe2 layers owing to the Cu-induced breaking of the centrosymmetry. Thus, this work sheds light on the exotic magnetic properties of layered materials that exhibit phenomena beyond weak interlayer interactions.

Ferromagnetic GdX (X = Cl, Br) Monolayers with Large Perpendicular Magnetic Anisotropy and High Curie Temperature

Two-dimensional (2D) ferromagnets with high Curie temperatures (TC) and large perpendicular magnetic anisotropy (PMA) are rare, but have great potential in the field of spintronics. The present work investigates the electronic and magnetic properties of GdX (X = Cl and Br) monolayers and the two layers of GdCl/GdBr heterojunctions by conducting in-depth theoretical calculations. As expected, both GdCl and GdBr monolayers are ferromagnetic and have large magnetic moments of ∼8 μB per Gd atom. Besides, they both show large PMA with magnetic anisotropy energies of 0.88 and 0.85 meV/unit cell and ultrahigh TC of 826 and 704 K, respectively. Significantly, they both have topological properties and spin-orbit-induced energy band reversion. In addition, we found two stable stacking configurations for the GdCl/GdBr bilayer heterojunction. The ultrahigh TC and topological properties are maintained in the two stacking configurations. Their easy magnetization axes shift from out-of-plane to in-plane directions as a result of the competition mainly between the Gd p and Gd d orbitals. These properties endow GdCl and GdBr monolayers with great potential for practical applications in the field of spintronic devices at the nanoscale.

Robust half-metallicity and tunable ferromagnetism in two-dimensional VClI2

Recent theoretical and experimental discoveries of two-dimensional (2D) ferromagnetic (FM) materials have sparked intense interest for their potential applications in spintronics. 2D FM materials with high spin polarization are extremely desirable for future low-dimensional spintronics. Half-metallicity plays a key role in the development of such devices. Here, we reported a new 2D nanomagnet VClI2 using the first-principles based density functional theory calculations. VClI2 shows an exciting half-metallic character with a wide half-metallic gap of 0.4 eV. The ground state favors ferromagnetic coupling with a Curie temperature Tc of 21 K. The half-metallicity with a FM ground state is further achieved by the application of an external strain and by the combined effects of the strain and the electric field. A phase transition from a half-metallic → semiconductor → metal was further observed under different stimuli with an antiferromagnetic ground state. At Ez=7.5 V/nm and in the presence of η=5% strain, the calculated Tc is estimated at 35 K, which shows a 67% increment than the Tc observed in the unstrained condition. The fascinating and unique properties suggest that VClI2 is a promising two-dimensional ferromagnetic half-metal, which can be useful for applications in future memory devices to enrich the 2D magnetic materials library.

Nonlocal Spin Valves Based on Graphene/Fe3GeTe2 van der Waals Heterostructures.

With recent advances in two-dimensional (2D) ferromagnets with enhanced Curie temperatures, it is possible to develop all-2D spintronic devices with high-quality interfaces using 2D ferromagnets. In this study, we have successfully fabricated nonlocal spin valves with Fe3GeTe2 (FGT) as the spin source and detector and multilayer graphene as the spin transport channel. The nonlocal spin transport signal was found to strongly depend on temperature and disappear at a temperature below the Curie temperature of the FGT flakes, which stemmed from the temperature-dependent ferromagnetism of FGT. The spin injection efficiency was estimated to be about 1%, close to that of conventional nonlocal spin valves with transparent contacts between ferromagnetic electrodes and the graphene channel. In addition, the spin transport signal was found to depend on the direction of the magnetic field and the magnitude of the current, which was due to the strong perpendicular magnetic anisotropy of FGT and the thermal effect, respectively. Our results provide opportunities to extend the applications of van der Waals heterostructures in spintronic devices.

Controlling Exchange Interactions and Emergent Magnetic Phenomena in Layered 3d‐Orbital Ferromagnets

AbstractLayered 3d‐orbital ferromagnet is an ideal research platform to experimentally achieve intrinsic 2D ferromagnetism and theoretically study the quantum nature of magnetic exchange interactions therein. A variety of magnetic phases can emerge from the strongly correlated feature of 3d‐orbital electrons, in which their exchange interactions can be effectively modulated by various kinds of external stimuli. Therefore, controlling the emergent magnetic phenomena of layered 3d‐orbital ferromagnets is significant in both fundamental science and practical applications. Considering the roles of magnetic exchange interactions, this review summarizes recent progress in controlling the emergent magnetic properties of layered 3d‐orbital ferromagnets by systematically introducing modulation methods, underlying mechanisms, and device applications. The existing challenges and future prospects for this research field are also outlined, shedding light on finding optimized magnetic materials, exploring powerful modulation techniques, and designing multifunctional new concept devices.

Dimension-dependent magnetic anisotropy for tunable anomalous Hall effect in transition metal dichalcogenides

Two-dimensional (2D) ferromagnetism at room temperature is highly desired in spintronic devices and applications. Recently, ${\mathrm{CrTe}}_{2}$ film has been successfully synthesized. Bulk ${\mathrm{CrTe}}_{2}$ has in-plane magnetic anisotropy (MA), and the Curie temperature reaches up to 300 K. When the dimensions are down to two, MA switches to out-of-plane. However, the mechanism of MA transition from in-plane to out-of-plane remains unknown. Here, we investigate the switching of MA in ${\mathrm{CrTe}}_{2}$ by second-order perturbation theory. The MA energy (MAE) originates from competition between ${p}_{z}/{p}_{y}$ and ${p}_{x}/{p}_{y}$ orbital hybridization, which contributes to out-of-plane and in-plane MA, respectively. The ${p}_{x}/{p}_{y}$ orbital hybridization, induced by van der Waals force, is absent in the monolayer. Moreover, the out-of-plane MA of monolayer ${\mathrm{CrTe}}_{2}$ breaks mirror symmetry, producing an anomalous Hall effect. Slight charge doping is significant to achieve a tunable anomalous Hall effect. Based on charge doping, we design a spintronic anomalous Hall device by taking advantage of the easily controllable properties of ${\mathrm{CrTe}}_{2}$. This highly thickness-dependent magnetism provides a perspective to control the magnetic properties of 2D materials.

Revealing the Origin of Time-Reversal Symmetry Breaking in Fe-Chalcogenide Superconductor FeTe_{1-x}Se_{x}.

Recently, evidence has emerged in the topological superconductor Fe-chalcogenide FeTe_{1-x}Se_{x} for time-reversal symmetry breaking (TRSB), the nature of which has strong implications on the Majorana zero modes (MZM) discovered in this system. It remains unclear, however, whether the TRSB resides in the topological surface state (TSS) or in the bulk, and whether it is due to an unconventional TRSB superconducting order parameter or an intertwined order. Here, by performing in superconducting FeTe_{1-x}Se_{x} crystals both surface-magneto-optic-Kerr effect measurements using a Sagnac interferometer and bulk magnetic susceptibility measurements, we pinpoint the TRSB to the TSS, where we also detect a Dirac gap. Further, we observe surface TRSB in nonsuperconducting FeTe_{1-x}Se_{x} of nominally identical composition, indicating that TRSB arises from an intertwined surface ferromagnetic (FM) order. The observed surface FM bears striking similarities to the two-dimensional (2D) FM found in 2D van der Waals crystals, and is highly sensitive to the exact chemical composition, thereby providing a means for optimizing the conditions for Majorana particles that are useful for robust quantum computing.

Ultrathin high-temperature ferromagnetic rare-earth films: GdScGe and GdScSi monolayers

Two-dimensional (2D) ferromagnetism with robust room-temperature ferromagnetism has sparked intense interest for future miniature information storage devices. However, most 2D ferromagnetic materials have a low Curie temperature. Here, by using density functional theory, two rare-earth monolayers, the GdScSi monolayer and the GdScGe monolayer, were predicted, in which these two monolayers exhibit ferromagnetic orders with large magnetic moments of approximately 7 μB/Gd. Monte Carlo simulations predict Curie temperatures of approximately 470 K and 495 K for the 2D GdScSi monolayer and the GdScGe monolayer, respectively. The spin band calculations show that they are metal. In addition, these two monolayers exhibit dynamical, mechanical, and thermal stabilities. The combination of these novel magnetic properties makes these 2D ferromagnetic crystals promising candidates for high-efficiency spintronic applications.

Electrical Interrogation of Thickness‐Dependent Multiferroic Phase Transitions in the 2D Antiferromagnetic Semiconductor NiI2

Abstract2D magnetic materials hold promise for quantum and spintronic applications. 2D antiferromagnetic materials are of particular interest due to their relative insensitivity to external magnetic fields and higher switching speeds compared to 2D ferromagnets. However, their lack of macroscopic magnetization impedes detection and control of antiferromagnetic order, thus motivating magneto‐electrical measurements for these purposes. Additionally, many 2D magnetic materials are ambient‐reactive and electrically insulating or highly resistive below their magnetic ordering temperatures, which imposes severe constraints on electronic device fabrication and characterization. Herein, these issues are overcome via a fabrication protocol that achieves electrically conductive devices from the ambient‐reactive 2D antiferromagnetic semiconductor NiI2. The resulting gate‐tunable transistors show band‐like electronic transport below the antiferromagnetic and multiferroic transition temperatures of NiI2, revealing a Hall mobility of 15 cm2 V−1 s−1 at 1.7 K. These devices also allow direct electrical probing of the thickness‐dependent multiferroic phase transition temperature of NiI2 from 59 K (bulk) to 28 K (monolayer).

Electric-field induced half-metallic properties in an experimentally synthesized CrSBr monolayer.

Two-dimensional (2D) half-metallic materials are highly desirable for nanoscale spintronic applications. Here, we propose a new mechanism that can achieve half-metallicity in 2D ferromagnetic (FM) materials with two-layer magnetic atoms by electric field tuning. We use a concrete example of an experimentally synthesized CrSBr monolayer to illustrate our proposal through first-principles calculations. It is found that half-metallic properties can be achieved in CrSBr within an appropriate electric field range, and the corresponding amplitude of electric field intensity can be realized experimentally. Janus monolayer Cr2S2BrI is constructed, which possesses a built-in electric field due to broken horizontal mirror symmetry. However, Cr2S2BrI without and with an applied external electric field is always a FM semiconductor. A possible memory device is also proposed based on the CrSBr monolayer. Our work will stimulate the application of 2D FM CrSBr in future spintronic nanodevices.

Room-temperature spin-valve devices based on Fe3GaTe2/MoS2/Fe3GaTe2 2D van der Waals heterojunctions.

The spin-valve effect has been the focus of spintronics over the last decades due to its potential for application in many spintronic devices. Two-dimensional (2D) van der Waals (vdW) materials are highly efficient to build spin-valve heterojunctions. However, the Curie temperatures (TC) of the vdW ferromagnetic (FM) 2D crystals are mostly below room temperature (∼30-220 K). It is very challenging to develop room-temperature, FM 2D crystal-based spin-valve devices. Here, we report room-temperature, FM 2D-crystal-based all-2D vdW Fe3GaTe2/MoS2/Fe3GaTe2 spin-valve devices. The magnetoresistance (MR) of the device was up to 15.89% at 2.3 K and 11.97% at 10 K, which are 4-30 times the MR of the spin valves of Fe3GeTe2/MoS2/Fe3GeTe2 and conventional NiFe/MoS2/NiFe. The typical spin valve effect showed strong dependence on the MoS2 spacer thickness in the vdW heterojunction. Importantly, the spin valve effect (0.31%) robustly existed even at 300 K with low working currents down to 10 nA (0.13 A cm-2). This work provides a general vdW platform to develop room-temperature, 2D FM-crystal-based 2D spin-valve devices.

Coexistence of ferromagnetism and charge density waves in monolayer LaBr2.

Charge density waves (CDWs), a common phenomenon of periodic lattice distortions, often suppress ferromagnetism in two-dimensional (2D) materials, hindering their magnetic applications. Here, we report a novel CDW that generates 2D ferromagnetism instead of suppressing it, through the formation of interstitial anionic electrons as the charge modulation mechanism. Via first-principles calculations and a low-energy effective model, we find that the highly symmetrical monolayer LaBr2 undergoes a 2 × 1 CDW transition to a magnetic semiconducting T' phase. Concurrently, the delocalized 5d1 electrons of La in LaBr2 redistribute and accumulate within the interstitial space in the T' phase, forming anionic electrons, also known as 2D electride or electrene. The strongly localized nature of anionic electrons promotes a Mott insulating state and full spin-polarization, while the overlap of their extended tails yields ferromagnetic direct exchange between them. Such transition introduces a new magnetic form of CDWs, offering promising opportunities for exploring novel fundamental physics and advanced spintronics applications.

Piezoelectric ferromagnetism in Janus monolayer YBrI: a first-principles prediction.

Coexistence of intrinsic ferromagnetism and piezoelectricity, namely piezoelectric ferromagnetism (PFM), is crucial to advance multifunctional spintronic technologies. In this work, we demonstrate that Janus monolayer YBrI is a PFM, which is dynamically, mechanically and thermally stable. The electronic correlation effects on the physical properties of YBrI are investigated by using generalized gradient approximation plus U (GGA+U) approach. For out-of-plane magnetic anisotropy, YBrI is a ferrovalley (FV) material, and its valley splitting is larger than 82 meV within the considered U range. The anomalous valley Hall effect (AVHE) can be achieved under an in-plane electric field. However, for in-plane magnetic anisotropy, YBrI is a common ferromagnetic (FM) semiconductor. When considering intrinsic magnetic anisotropy, the easy axis of YBrI is always in-plane, and its magnetic anisotropy energy (MAE) varies from 0.309 meV to 0.237 meV (U = 0.0 eV to 3.0 eV). However, the magnetization can be adjusted from the in-plane to out-of-plane direction by an external magnetic field, and then lead to the occurrence of valley polarization. Moreover, the missing centrosymmetry along with broken mirror symmetry results in both in-plane and out-of-plane piezoelectricity in the YBrI monolayer. At a typical U = 2.0 eV, the piezoelectric strain coefficient d11 is predicted to be -5.61 pm V-1, which is higher than or comparable with the ones of other known two-dimensional (2D) materials. The electronic and piezoelectric properties of YBrI can be effectively tuned by applying biaxial strain. For example, tensile strain can enhance valley splitting and d11 (absolute value). The predicted magnetic transition temperature of YBrI is higher than those of experimentally synthesized 2D FM materials CrI3 and Cr2Ge2Te6. Our findings of these distinctive properties could pave the way for designing multifunctional spintronic devices, and bring forward a new perspective for constructing 2D materials.

High-temperature ferromagnetism and strong π-conjugation feature in two-dimensional manganese tetranitride

Two-dimensional (2D) magnetic materials have attracted tremendous research interest because of the promising application in the next-generation microelectronic devices. Here, by the first-principles calculations, we propose a two-dimensional ferromagnetic material with high Curie temperature, manganese tetranitride MnN4 monolayer, which is a square-planar lattice made up of only one layer of atoms. The structure is demonstrated to be stable by the phonon spectra and the molecular dynamic simulations, and the stability is ascribed to the π–d conjugation between π orbital of N=N bond and d orbital of Mn. More interestingly, the MnN4 monolayer displays robust 2D ferromagnetism, which originates from the strong exchange couplings between Mn atoms due to the π–d conjugation. The high critical temperature of 247 K is determined by solving the Heisenberg model using the Monte Carlo method.

FIRST-PRINCIPLES STUDY OF MAGNETIC ANISOTROPY ENERGY IN TWO-DIMENSIONAL FERROMAGNETIC CrI3

First-principles calculations are increasingly crucial in searching for new materials with customized properties or new functionality. First-principles calculations are superior in speed and cost, and comparable to experiments in terms of accuracy. Two-dimensional (2D) ferromagnetism materials were successfully fabricated experimentally in atomic thin films of CrI3. 2D intrinsic ferromagnetism with perpendicular magnetic anisotropy energy (PMAE) is an encouraging applicant compatible with high-density magnetic storage applications. In this study, spin density functional calculations are investigated on the magnetic anisotropy energy (MAE) in 2D monolayer ferromagnetic CrI3 using a first-principles electronic structure calculation. We include the MAE part calculation from the magnetocrystalline anisotropy energy (MCAE) that comes from the spin-orbit coupling (SOC). In the present calculation, the MCAE part, in addition to a usual scheme of total energy (TE), was evaluated using a grand-canonical force theorem (GCFT) scheme. The MCAE of 2D monolayer ferromagnetic CrI3 is 1.7 meV/unit cell and verified it has an easy-axis perpendicular to the crystal plane, which is a good agreement with experimental measurement. In the latter scheme, employing GCFT, we evaluated atom-resolved, k-resolved, and atomic k-resolved analyses for MCAE can be performed. From the GCFT result, the Cr atom indicates that it is the primary origin of PMAE in the atom-resolved MCAE. The negative MCAE contribution is in points, and the positive MCAE is mainly placed at the line in the 2D first Brillouin zone. Our systematic calculation in this work may also help design an effective structure of monolayer CrI3 in new 2D material magnetic sensor and spintronic device designs.

Layer-Number-Independent Two-Dimensional Ferromagnetism in Cr3Te4

In a conventional magnetic material, a long-range magnetic order develops in three dimensions, and reducing a layer number weakens its magnetism. Here we demonstrate anomalous layer-number-independent ferromagnetism down to the two-dimensional (2D) limit in a metastable phase of Cr3Te4. We fabricated Cr3Te4 thin films by molecular-beam epitaxy and found that Cr3Te4 could host two distinct ferromagnetic phases characterized with different Curie temperatures (TC). One is the bulk-like "high-TC phase" showing room-temperature ferromagnetism, which is consistent with previous studies. The other is the metastable "low-TC phase" with TC ≈ 160 K, which exhibits a layer-number-independent TC down to the 2D limit in marked contrast with the conventional high-TC phase, demonstrating a purely 2D nature of its ferromagnetism. Such significant differences between two distinct phases could be attributed to a small variation in the doping level, making this material attractive for future ultracompact spintronics applications with potential gate-tunable room-temperature 2D ferromagnetism.