Unusual Dzyaloshinskii-Moriya Interaction in Graphene/Fe3GeTe2 Van der Waals Heterostructure.

Dzyaloshinskii-Moriya interaction (DMI) is shown to induce a topologically protected chiral spin texture in magnetic/nonmagnetic heterostructures. In the context of van der Waals spintronic devices, graphene emerges as an excellent candidate material. However, due to its negligible spin-orbit interaction, inducing DMI to stabilize topological spins when coupled to 3d-ferromagnets remains challenging. Here, it is demonstrated that, despite these challenges, a sizeable Rashba-type spin splitting followed by significant DMI is induced in graphene/Fe3GeTe2. This is made possible due to an interfacial electric field driven by charge asymmetry together with the broken inversion symmetry of the heterostructure. These findings reveal that the enhanced DMI energy parameter, resulting from a large effective electron mass in Fe3GeTe2, remarkably contributes to stabilizing non-collinear spins below the Curie temperature, overcoming the magnetic anisotropy energy. These results are supported by the topological Hall effect, which coexists with the non-trivial breakdown of Fermi liquid behavior, confirming the interplay between spins and non-trivial topology. This work paves the way toward the design and control of interface-driven skyrmion-based devices.

Boosting the Curie temperature of GaN monolayer through van der Waals heterostructures.

The pursuit of van der Waals (vdW) heterostructures with high Curie temperature and strong perpendicular magnetic anisotropy (PMA) is vital to the advancement of next generation spintronic devices. First-principles calculations are used to study the electronic structures and magnetic characteristics of GaN/VS2vdW heterostructure under biaxial strain and electrostatic doping. Our findings show that a ferromagnetic ground state with a remarkable Curie temperature (477 K), much above room temperature, exists in GaN/VS2vdW heterostructure and 100% spin polarization efficiency. Additionally, GaN/VS2vdW heterostructure still maintains PMA under biaxial strain, which is indispensable for high-density information storage. We further explore the electron, magnetic, and transport properties of VS2/GaN/VS2vdW sandwich heterostructure, where the magnetoresistivity can reach as high as 40%. Our research indicates that the heterostructure constructed by combining the ferromagnet VS2and the non-magnetic semiconductor GaN is a promising material for vdW spin valve devices at room temperature.

Electronic Structure of Above-Room-Temperature van der Waals Ferromagnet Fe3GaTe2.

Fe3GaTe2, a recently discovered van der Waals ferromagnet, demonstrates intrinsic ferromagnetism above room temperature, necessitating a comprehensive investigation of the microscopic origins of its high Curie temperature (TC). In this study, we reveal the electronic structure of Fe3GaTe2 in its ferromagnetic ground state using angle-resolved photoemission spectroscopy and density functional theory calculations. Our results establish a consistent correspondence between the measured band structure and theoretical calculations, underscoring the significant contributions of the Heisenberg exchange interaction (Jex) and magnetic anisotropy energy to the development of the high-TC ferromagnetic ordering in Fe3GaTe2. Intriguingly, we observe substantial modifications to these crucial driving factors through doping, which we attribute to alterations in multiple spin-splitting bands near the Fermi level. These findings provide valuable insights into the underlying electronic structure and its correlation with the emergence of high-TC ferromagnetic ordering in Fe3GaTe2.

Strain Tunability of Perpendicular Magnetic Anisotropy in van der Waals Ferromagnets VI3.

Layered ferromagnets with strong magnetic anisotropy energy (MAE) have special applications in nanoscale memory elements in electronic circuits. Here, we report a strain tunability of perpendicular magnetic anisotropy in van der Waals (vdW) ferromagnets VI3 using magnetic circular dichroism measurements. For an unstrained flake, the M-H curve shows a rectangular-shaped hysteresis loop with a large coercivity (1.775 T at 10 K) and remanent magnetization. Furthermore, the coercivity can be enhanced to a maximum of 2.6 T under a 3.8% external in-plane tensile strain. Our DFT calculations show that the increased MAE under strain contributes to the enhancement of coercivity. Meanwhile, the strain tunability on the coercivity of CrI3, with a similar crystal structure, is limited. The main reason is the strong spin-orbit coupling in V3+ in VI6 octahedra in comparison with that in Cr3+. The strain tunability of coercivity in VI3 flakes highlights its potential for integration into vdW heterostructures.

OsPd bimetallic dimer pushes the limit of magnetic anisotropy in atom-sized magnets for data storage.

The growing gap between the volume of digital data being created and the extent of available storage capacities stimulates intensive research into surface-supported, well-ordered array of atom-sized magnets that represents the ultimate limit of magnetic data storage. Anchoring transition-metal heterodimers in vacancy defects in the graphene lattice has been identified as a vivid strategy to achieve large magnetic anisotropy energy (MAE) up to 80 meV with an easy axis aligned along the dimer bond. In this paper we have made a significant leap forward finding out MAE of 119 meV for an OsPt dimer and 170 meV for an OsPd dimer bound to a single nitrogen-decorated vacancy defect. The system with the highest MAE and with the theoretical storage density of ∼490 Tb·inch-2pushes the current limit of theoretical blocking temperature in graphene-supported transition-metal dimers from ∼20 to ∼44 K assuming the relaxation time of 10 years. The mechanism of the enhanced MAE is discussed.

OsPd bimetallic dimer pushes the limit of magnetic anisotropy in atom-sized magnets for data storage.

The growing gap between the volume of digital data being created and the extent of available storage capacities stimulates intensive research into surface-supported, well-ordered array of atom-sized magnets that represents the ultimate limit of magnetic data storage. Anchoring transition metal heterodimers in vacancy defects in the graphene lattice has been identified as a vivid strategy to achieve large magnetic anisotropy energy (MAE) up to 80 meV with an easy axis aligned along the dimer bond. In this paper we have made a significant leap forward finding out MAE of 119 meV for an OsPt dimer and 170 meV for an OsPd dimer bound to a single nitrogen-decorated vacancy defect. The system with the highest MAE and with the theoretical storage density of 490 Tb inch-2pushes the current limit of theoretical blocking temperature in graphene-supported transition-metal dimers from ~20 K to ~44 K assuming the relaxation time of 10 years. The mechanism of the enhanced MAE is discussed.

Large magnetic anisotropy in an OsIr dimer anchored in defective graphene.

Single-atom magnets represent the ultimate limit of magnetic data storage. The identification of substrates that anchor atom-sized magnets firmly and, thus, prevent their diffusion and large magnetic anisotropy has been at the centre of intense research efforts for a long time. Using density functional theory we show the binding of transition metal (TM) atoms in defect sites in the graphene lattice: single vacancy and double vacancy, both pristine and decorated by pyridinic nitrogen atoms, are energetically more favourable than away from the centre of defects, which could be used for engineering the position of TMs with atomic precision. Relativistic calculations revealed magnetic anisotropy energy (MAE) of ∼10 meV for Ir@NSV with an easy axis parallel to the graphene plane. MAE can be remarkably boosted to 50 meV for OsIr@NSV with the easy axis perpendicular to the graphene plane, which paves the way to the storage density of ∼490 Tb/inch2with the blocking temperature of 14 K assuming the relaxation time of 10 years. Magnetic anisotropy is discussed based on the relativistic electronic structures. The influence of an orbital-dependent on-site Coulomb repulsionUand a non-local correlation functional optB86b-vdW on MAE is also discussed.

Zero-Point Spin-Fluctuations of Single Adatoms.

Stabilizing the magnetic signal of single adatoms is a crucial step toward their successful usage in widespread technological applications such as high-density magnetic data storage devices. The quantum mechanical nature of these tiny objects, however, introduces intrinsic zero-point spin-fluctuations that tend to destabilize the local magnetic moment of interest by dwindling the magnetic anisotropy potential barrier even at absolute zero temperature. Here, we elucidate the origins and quantify the effect of the fundamental ingredients determining the magnitude of the fluctuations, namely, the (i) local magnetic moment, (ii) spin-orbit coupling, and (iii) electron-hole Stoner excitations. Based on a systematic first-principles study of 3d and 4d adatoms, we demonstrate that the transverse contribution of the fluctuations is comparable in size to the magnetic moment itself, leading to a remarkable ≳50% reduction of the magnetic anisotropy energy. Our analysis gives rise to a comprehensible diagram relating the fluctuation magnitude to characteristic features of adatoms, providing practical guidelines for designing magnetically stable nanomagnets with minimal quantum fluctuations.

Chern half metals: a new class of topological materials to realize the quantum anomalous Hall effect.

New topological insulators that demonstrate the quantum anomalous Hall effect (QAHE) are a cutting-edge research topic in condensed matter physics and materials science. So far, the QAHE has been observed only in Cr-doped (Bi,Sb)2Te3 at extremely low temperature. Therefore, it is important to find new materials with large topological band gap and high thermal stability for the realization of the QAHE. On the basis of first-principles and tight-binding model calculations, we discovered a new class of topological phase, Chern half metal, which manifests the QAHE in one spin channel while is metallic in the other spin channel, in Co or Rh deposited graphene. The QAHE is robust in these sytems for the adatom coverage ranging from 2% to 6%. Meanwhile, these systems have large perpendicular magnetic anisotropy energies of 5.3 and 11.5 meV, necessary for the observation of the QAHE at reasonably high temperature.

Transformation of in-plane to out-of-plane anisotropy in MnBi alloy for permanent magnet application: a First-principles study.

The low-temperature phase (LTP) MnBi exhibits remarkable ferromagnetic properties at room temperature. However, below its Curie temperature ( T C ), a phase transition occurs around 613 K due to diffusion of Mn into interstitial sites, raising concerns about its structural and magnetic properties. Furthermore, the presence of in-plane anisotropy in LTP-MnBi alloy at low temperatures raises concerns about its suitability for use in permanent magnet applications, even at higher temperature. Therefore, this study examines the structural and magnetic properties of pure LTP-MnBi and its successive Ni-doped and Fe-substituted alloys using first-principles study based on density functional theory (DFT). To prevent Mn diffusion into interstitial sites, Ni doping is employed. Additionally, the incorporation of Ni successfully addresses the in-plane anisotropy issue in LTP-MnBi, transforming it into out-of-plane anisotropy. Moreover, we explored the potential advantages of substituting Fe for one of Mn site. This substitution aims to improve the observed dynamical instability in Ni-doped alloy and to further enhanced the magnetocrystalline anisotropy energy (MAE) of the material, resulting in an MAE of 3.21 MJ/m3, along with a T C of 523 K. Therefore, the coexistence of high MAE and moderate T C in the Mn0.5Fe0.5Bi-Ni alloy presents viable option for its application in permanent magnet technology.

Two-Dimensional Room-Temperature Magnetism in Janus Mn2I3S3 and Cr2I3Se3 Monolayers with Tunable Magnetic Properties by Strain Engineering.

Exploring room-temperature intrinsic magnetism in two-dimensional (2D) materials for nanoscale spintronic devices has garnered significant interest. Achieving a high Curie temperature and substantial spin polarization in 2D ferromagnetic materials remains challenging. Drawing inspiration from the substantial enhancement of the Curie temperature observed in ferromagnetic CrIS monolayers by manipulating the covalent nature of Cr-S bonds, our study systematically delves into the electronic structure and magnetic properties of Janus M2X3Y3 (M = V, Cr, Mn, Fe, and Co; X = Cl, Br, I; Y = S, Se, and Te) monolayers through first-principles calculations. Our findings reveal that 15 kinds of these monolayers exhibit dynamic and thermodynamic stability while displaying diverse electronic and ferromagnetic characteristics. Notably, Mn2I3S3 demonstrates half-metallicity and in-plane magnetic anisotropy, while Cr2I3Se3 exhibits a half-semiconductor and perpendicular magnetic anisotropy. Consequently, Mn2I3S3 transforms from in-plane to perpendicular magnetic anisotropy through strain manipulation. Cr2I3Se3, under strain, transforms from a half-semiconductor to a bipolar magnetic semiconductor. The strong coupling caused by the M-Y bonds makes them have a Curie temperature higher than room temperature. The unique magnetic properties exhibited by the 2D Janus Mn2I3S3 and Cr2I3Se3 magnets hold promise for applications in spintronics. Our study provides a foundational understanding for future experimental explorations in this exciting research area.

Large thermoelectric transport in magnetically coupled CrI3/1T-MoS2vdW heterostructure via spin-charge interconversion.

Low-dimensional materials with prominent thermoelectric (TE) effect play a pivotal role in realizing state-of-the-art nanoscale TE devices. The fusion of TE effect with the magnetism through seamless integration of TE and magnetic materials in the 2D limit offers access to control longitudinal as well as transverse TE properties via magnetic proximity effect. Herein, we design a van der Waals (vdW) heterostructure of metallic 1T-MoS2with promising TE properties and a layer-dependent magnetic CrI3material. The result highlights exotic electronic and magnetic configurations of the designed monolayer-CrI3/1T-MoS2vdW heterostructure, which show magnetically-coupled TE characteristics. The observed remarkable magnetic proximity stems from large magnetic anisotropy energy and spin polarization, which are found to be 2.21 meV Cr-1and 12.30%, respectively. To this end, the semiconducting CrI3layer with intrinsic magnetism leads to efficient control and tunability of the observed spin-correlated anomalous Nernst effect. Moreover, a large dimensionless figure of merit of ∼6 and a power factor of∼3.8×1011/τ∘ Wm-1K-2s-1near the Fermi level at 300 K endorse the rejuvenated TE effect. The strong relativistic spin-orbit coupling validates the significant correlation of TE properties with intrinsic magnetic configuration. The present study underscores the significance of the magnetic proximity-governed TE effect in vdW heterostructures to engineer low-dimensional TE devices.

Hole-Doping-Induced Perpendicular Magnetic Anisotropy and High Curie Temperature in a CrSX (X = Cl, Br, I) Semiconductor Monolayer.

A large perpendicular magnetic anisotropy and a high Curie temperature (TC) are crucial for the application of two-dimensional (2D) intrinsic ferromagnets to spintronic devices. Here, we investigated the electronic and magnetic properties of carrier-doped Van der Waals layered CrSX (X = Cl, Br, I) ferromagnets using first-principles calculations. It was found that hole doping can increase the magnitude of the magnetic anisotropy energy (MAE) and change the orientation of the easy magnetization axis at small doping amounts of 2.37 × 1013, 3.98 × 1012, and 3.33 × 1012/cm2 for CrSCl, CrSBr, and CrSI monolayers, respectively. The maximum values of the MAE reach 57, 133, and 1597 µeV/u.c. for the critical hole-doped CrSCl, CrSBr, and CrSI with spin orientation along the (001) direction, respectively. Furthermore, the Fermi energy level of lightly hole-doped CrSX (X = Cl, Br, I) moves into the spin-up valence band, leading to the CrSX (X = Cl, Br, I) magnetic semiconductor monolayer becoming first a half-metal and then a metal. In addition, the TC can also be increased up to 305, 317, and 345 K for CrSCl, CrSBr, and CrSI monolayers at doping amounts of 5.94 × 1014, 5.78 × 1014, and 5.55 × 1014/cm2, respectively. These properties suggest that the hole-doping process can render 2D CrSX (X = Cl, Br, I) monolayers remarkable materials for application to electrically controlled spintronic devices.

Two dimensional Zr2CO2/H-FeCl2van der Waals heterostructures with tunable band gap, potential difference and magnetic anisotropy.

Two dimensional (2D) van der Waals (vdW) heterostructures have potential applications in novel low dimensional spintronic devices due to their unique electronic and magnetic properties. Here, the electronic and magnetic properties of 2D Zr2CO2/H-FeCl2heterostructures are calculated by first principles calculations. The 2D Zr2CO2/H-FeCl2heterostructures are magnetic semiconductor. The electronic structure and magnetic anisotropy of Zr2CO2/H-FeCl2heterostructure can be regulated by the biaxial strain and external electric field. The band gap and potential difference of Zr2CO2/H-FeCl2heterostructure can be affected by in-plane biaxial strain. At a compressive strain of -8%, the Zr2CO2/H-FeCl2heterostructure becomes metallic. All of the Zr2CO2/H-FeCl2heterostructures are magnetic with in-plane magnetic anisotropy (IMA). The Zr2CO2/H-FeCl2heterostructure is a semiconductor at the electric field from -0.5 V Å-1to +0.5 V Å-1. Furthermore, Zr2CO2/H-FeCl2heterostructure shows IMA at the negative electric field, while it shows perpendicular magnetic anisotropy at the positive electric field. These results show that Zr2CO2/H-FeCl2heterostructure has potential applications in multifunctionalnanoelectronic devices.

Conversation from antiferromagnetic MnBr2 to ferromagnetic Mn3Br8 monolayer with large MAE.

A pressing need in low energy spintronics is two-dimensional (2D) ferromagnets with Curie temperature above the liquid-nitrogen temperature (77 K), and sizeable magnetic anisotropy. We studied Mn3Br8 monolayer which is obtained via inducing Mn vacancy at 1/4 population in MnBr2 monolayer. Such defective configuration is designed to change the coordination structure of the Mn-d5 and achieve ferromagnetism with sizeable magnetic anisotropy energy (MAE). Our calculations show that Mn3Br8 monolayer is a ferromagnetic (FM) half-metal with Curie temperature of 130 K, large MAE of - 2.33 meV per formula unit, and atomic magnetic moment of 13/3µB for the Mn atom. Additionally, Mn3Br8 monolayer maintains to be FM under small biaxial strain, whose Curie temperature under 5% compressive strain is 160 K. Additionally, both biaxial strain and carrier doping make the MAE increases, which mainly contributed by the magneto-crystalline anisotropy energy (MCE). Our designed defective structure of MnBr2 monolayer provides a simple but effective way to achieve ferromagnetism with large MAE in 2D materials.

Magnetic structure and exchange interactions in pyrrhotite end member minerals: hexagonal FeS and monoclinic Fe7S8.

Iron mono-sulphides, or pyrrhotites, are minerals present in the Earth's crust and mantle as well as major magnetic constituents of several classes of meteorites, thus are of interest to a wide range of disciplines including geology, geophysics, geochemistry, and material science. Despite displaying diverse magnetic properties as a result of iron vacancy ordering, the underlying exchange mechanism has not been quantified. This study presents an examination of the electronic and magnetic properties for the two pyrrhotite group end members, hexagonal FeS and monoclinic Fe7S8(4C superstructure) by means of density functional theory coupled with a Heisenberg magnetic model. The easy magnetization axes of FeS and Fe7S8are found to be positioned along the crystallographicc-direction and at an angle of 56° to thec-direction, respectively. The magnetic anisotropy energy in Fe7S8is greatly increased as a consequence of the vacancy framework when compared to FeS. The main magnetic interaction, in both compounds, is found to be the isotropic exchange interaction favouring antiferromagnetic alignment between nearest-neighbouring spins. The origin of the exchange interaction is elucidated further following the Goodenough-Kanamori-Anderson rules. The antisymmetric spin exchange is found to have a minor effect in both compounds. The theoretical findings presented in this work thus help to further resolve some of the ambiguities in the magnetic features of pyrrhotites.