Antiferromagnetic Insulator Research Articles

Multi-state data storage in a two-dimensional stripy antiferromagnet implemented by magnetoelectric effect

A promising approach to the next generation of low-power, functional, and energy-efficient electronics relies on novel materials with coupled magnetic and electric degrees of freedom. In particular, stripy antiferromagnets often exhibit broken crystal and magnetic symmetries, which may bring about the magnetoelectric (ME) effect and enable the manipulation of intriguing properties and functionalities by electrical means. The demand for expanding the boundaries of data storage and processing technologies has led to the development of spintronics toward two-dimensional (2D) platforms. This work reports the ME effect in the 2D stripy antiferromagnetic insulator CrOCl down to a single layer. By measuring the tunneling resistance of CrOCl on the parameter space of temperature, magnetic field, and applied voltage, we verified the ME coupling down to the 2D limit and probed its mechanism. Utilizing the multi-stable states and ME coupling at magnetic phase transitions, we realize multi-state data storage in the tunneling devices. Our work not only advances the fundamental understanding of spin-charge coupling, but also demonstrates the great potential of 2D antiferromagnetic materials to deliver devices and circuits beyond the traditional binary operations.

Interplay between Magnetism and Topology: Large Topological Hall Effect in an Antiferromagnetic Topological Insulator, EuCuAs.

Magnetic interactions in combination with nontrivial band structures can give rise to several exotic physical properties such as a large anomalous Hall effect, the anomalous Nernst effect, and the topological Hall effect (THE). Antiferromagnetic (AFM) materials exhibit the THE due to the presence of nontrivial spin structures. EuCuAs crystallizes in a hexagonal structure with an AFM ground state (Néel temperature ∼ 16 K). In this work, we observe a large topological Hall resistivity of ∼7.4 μΩ-cm at 13 K which is significantly higher than the giant topological Hall effect of Gd2PdSi3 (∼3 μΩ-cm). Neutron diffraction experiments reveal that the spins form a transverse conical structure during the metamagnetic transition, resulting in the large THE. In addition, by controlling the magnetic ordering structure of EuCuAs with an external magnetic field, several fascinating topological states such as Dirac and Weyl semimetals have been revealed. These results suggest the possibility of spintronic devices based on antiferromagnets with tailored noncoplanar spin configurations.

Crystal structure and physical properties of layered Na[formula omitted]Fe[formula omitted]S[formula omitted

Layered iron oxysulfide Na2Fe2S2O serves as a cathode material for Na-ion batteries as well as a possible parent compound of novel superconductors. Here we report the crystal structure and physical properties on the basis of our successful synthesis of the high-purity sample. Na2Fe2S2O crystallizes in an anti-K2NiF4-type structure, which gives rise to the characteristic [Fe2S2O]2− block layers. The physical property measurements indicate that it is an antiferromagnetic insulator with a Néel temperature of TN=91.5 K and an energy gap no less than 0.43 eV. Evidence of two-dimensional short-range spin correlations above TN is given by the magnetic and specific-heat measurements. Our structural correlation analysis suggests that the Fe–S bond distance dominantly determines TN.

Terahertz Spin Current Pulses in Antiferromagnetic Oxide: The Role of Vacancy‐Induced Ferromagnetism

Antiferromagnetic oxides have attracted increasing attention for their outstanding peculiarities in spintronics. Crystal lattice defects that are present in antiferromagnetic oxides can influence their physical properties, such as vacancy‐induced ferromagnetism. Meanwhile, the generation and manipulation of ultrafast spin currents of antiferromagnetic insulators are highly desired. Although the generation and detection of terahertz spin current pulses in antiferromagnetic oxides have been realized, the effect of vacancy‐induced ferromagnetism on spin current in antiferromagnetic oxides is not yet known. Herein, the role of vacancy‐induced ferromagnetism on the terahertz spin current in antiferromagnetic nickel oxide thin films is reported. Structural and magnetic characterizations reveal that nickel vacancies effectively break the strong antiferromagnetic exchange coupling, giving rise to the coexistence of antiferromagnetism and ferromagnetism in NiO thin films. Notably, the enhancement of terahertz radiation associated with the photo‐induced ultrafast spin current of NiO thin film with the strongest ferromagnetism is the most significant. Besides, the nonlinear susceptibility tensor parameters related to the antiferromagnetic property of NiO thin films also change distinctly. The findings indicate that the defects of antiferromagnetic materials play a decisive role in the application of antiferromagnetic spintronics in the terahertz field.

Superexchange Interactions and Magnetic Anisotropy in MnPSe3 Monolayer

Two-dimensional van der Waals magnetic materials are of great current interest for their promising applications in spintronics. Using density functional theory calculations in combination with the maximally localized Wannier functions method and the magnetic anisotropy analyses, we study the electronic and magnetic properties of MnPSe3 monolayer. Our results show that it is a charge transfer antiferromagnetic (AF) insulator. For this Mn2+ 3d 5 system, although it seems straightforward to explain the AF ground state using the direct exchange, we find that the nearly 90° Mn–Se–Mn charge transfer type superexchange plays a dominant role in stabilizing the AF ground state. Moreover, our results indicate that, although the shape anisotropy favors an out-of-plane spin orientation, the spin-orbit coupling (SOC) leads to the experimentally observed in-plane spin orientation. We prove that the actual dominant contribution to the magnetic anisotropy comes from the second-order perturbation of the SOC, by analyzing its distribution over the reciprocal space. Using the AF exchange and anisotropy parameters obtained from our calculations, our Monte Carlo simulations give the Néel temperature T N = 47 K for MnPSe3 monolayer, which agrees with the experimental 40 K. Furthermore, our calculations show that under a uniaxial tensile (compressive) strain, Néel vector would be parallel (perpendicular) to the strain direction, which well reproduces the recent experiments. We also predict that T N would be increased by a compressive strain.

Observation of the Unidirectional Magnetoresistance in Antiferromagnetic Insulator Fe2O3/Pt Bilayers

AbstractUnidirectional magnetoresistance (UMR) has been observed in a variety of stacks with ferromagnetic/spin Hall material bilayer structures. In this work, UMR in antiferromagnetic insulator Fe2O3/Pt structure is reported. The UMR has a negative value, which is related to interfacial Rashba coupling and band splitting. Thickness‐dependent measurement reveals a potential competition between UMR and the unidirectional spin Hall magnetoresistance (USMR). This work reveals the existence of UMR in antiferromagnetic insulators/heavy metal bilayers and broadens the way for the application of antiferromagnet‐based spintronic devices.

Renormalization of antiferromagnetic magnons by superconducting condensate and quasiparticles

The ability to modify and tune the spin-wave dispersion is one of the most important requirements for engineering of magnonic networks. In this study we demonstrate the promise of synthetic thin-film hybrids composed of an antiferromagnetic insulator (AF) and a normal (N) or superconducting (S) metal for tuning and modifying the spin-wave dispersion in antiferromagnetic insulators. The key ingredient is the uncompensated magnetic moment at the AF/S(N) interface, which induces an effective exchange field in the adjacent metal via the interface exchange interaction. The exchange field spin polarizes quasiparticles in the metal and induces spinful triplet Cooper pairs screening the magnon. The quasiparticle and Cooper pair polarization renormalizes the magnon dispersion. The renormalization results in the splitting of the otherwise degenerate AF magnon modes with no need to apply a magnetic field. It is also proposed that measurements of the renormalized dispersion relations can provide the amplitude of the effective exchange field induced by the AF in the adjacent metal.

Onset of Antiferromagnetic Insulator‐to‐Ferromagnetic Half Metal‐to‐Antiferromagnetic Metal Transitions in La1−xCaxCrO3 and their Microscopic Origin

The magnetic ground state of LaCrO3 and CaCrO3 solid solution is investigated in the complete miscibility range, that is, La1−xCaxCrO3 with 0 ≤ x ≤ 1 at the interval of x = 0.25 to understand the magnetic phase transitions with Ca substitutional fraction. The density functional theory is used with Hubbard correction to account for Cr exchange interaction. The isostructural La1−xCaxCrO3 system exhibits antiferromagnetic insulator (x = 0, i.e., LaCrO3) to ferromagnetic half metal (x = 0.75, i.e., La0.25Ca0.75CrO3) to antiferromagnetic metal (x = 1, i.e., CaCrO3) phase transitions. Cr changes its oxidation state from 3+ in LaCrO3 to 4+ in CaCrO3, showing both 3+ and 4+ states for intermediate compositions. Interestingly, the introduction of Hubbard energy U and Ca substitution affects Cr–O hybridization, as observed in partial density of states. A compositional phase diagram with magnetic ground state is presented for the La1−xCaxCrO3 (0 ≤ x ≤ 1) system.

Reversible metal-insulator transition in SrIrO3 ultrathin layers by field effect control of inversion symmetry breaking

SrIrO3 is a correlated semimetal with narrow t2g d-bands of strong mixed orbital character resulting from the interplay of the spin-orbit interaction due to heavy iridium atoms and the band folding induced by the lattice structure. In ultrathin layers, inversion symmetry breaking, occurring naturally due to the presence of the substrate, opens new orbital hopping channels, which in presence of spin-orbit interaction causes deep modifications in the electronic structure. Here, we show that in SrIrO3 ultrathin films the effect of inversion symmetry breaking on the band structure can be externally manipulated in a field effect experiment. We further prove that the electric field toggles the system reversibly between a metallic and an insulating state with canted antiferromagnetism and an emergent anomalous Hall effect. This is achieved through the spin-orbit driven coupling of the electric field generated in an ionic liquid gate to the electronic structure, where the electric field controls the band structure rather than the usual band filling, thereby enabling electrical control of the effective role of electron correlations. The externally tunable antiferromagnetic insulator, rooted in the strong spin-orbit interaction of iridium, may inspire interesting applications in spintronics.

Observation of the Nonreciprocal Magnon Hanle Effect.

The precession of magnon pseudospin about the equilibrium pseudofield, the latter capturing the nature of magnonic eigenexcitations in an antiferromagnet, gives rise to the magnon Hanle effect. Its realization via electrically injected and detected spin transport in an antiferromagnetic insulator demonstrates its high potential for devices and as a convenient probe for magnon eigenmodes and the underlying spin interactions in the antiferromagnet. Here, we observe a nonreciprocity in the Hanle signal measured in hematite using two spatially separated platinum electrodes as spin injector or detector. Interchanging their roles was found to alter the detected magnon spin signal. The recorded difference depends on the applied magnetic field and reverses sign when the signal passes its nominal maximum at the so-called compensation field. We explain these observations in terms of a spin transport direction-dependent pseudofield. The latter leads to a nonreciprocity, which is found to be controllable via the applied magnetic field. The observed nonreciprocal response in the readily available hematite films opens interesting opportunities for realizing exotic physics predicted so far only for antiferromagnets with special crystal structures.

Magneto-optical Kerr and Faraday effects in bilayer antiferromagnetic insulators

Control and detection of antiferromagnetic topological materials are challenging since the total magnetization vanishes. Here we investigate the magneto-optical Kerr and Faraday effects in bilayer antiferromagnetic insulator MnBi2Te4. We find that by breaking the combined mirror symmetries with either perpendicular electric field or external magnetic moment, Kerr and Faraday effects occur. Under perpendicular electric field, antiferromagnetic topological insulators (AFMTI) show sharp peaks at the interband transition threshold, whereas trivial insulators show small adjacent positive and negative peaks. Gate voltage and Fermi energy can be tuned to reveal the differences between AFMTI and trivial insulators. We find that AFMTI with large antiferromagnetic order can be proposed as a pure magneto-optical rotator due to sizable Kerr (Faraday) angles and vanishing ellipticity. Under external magnetic moment, AFMTI and trivial insulators are significantly different in the magnitude of Kerr and Faraday angles and ellipticity. For the qualitative behaviors, AFMTI shows distinct features of Kerr and Faraday angles when the spin configurations of the system change. These phenomena provide new possibilities to optically detect and manipulate the layered topological antiferromagnets.

Doping tuned anomalous Hall effect in the van der Waals magnetic topological phases Mn(Sb1 − x Bi x )4Te7

The van der Waals (vdW) MnSb4Te7 is a newly synthesized antiferromagnetic (AFM) topological insulator hosting a robust axion insulator state irrelative to the specific spin structure. However, the intrinsic hole doped character of MnSb4Te7 makes the Fermi level far away from the Dirac point of about 180 meV, which is unfavorable for the exploration of exotic topological properties such as the quantum anomalous Hall effect (QAHE). To shift up the Fermi level close to the Dirac point, the strategy of partially replacing Sb with Bi as Mn(Sb1−x Bi x )4Te7 was tried and the magnetotransport properties, in particular, the anomalous Hall effect, were measured and analyzed. Through the electron doping, the anomalous Hall conductance σ AH changes from negative to positive between x = 0.3 and 0.5, indicative of a possible topological transition. Besides, a charge neutrality point (CNP) also appears between x = 0.6 and 0.7. The results would be instructive for further understanding the interplay between nontrivial topological states and the magnetism, as well as for the exploration of exotic topological properties.

Vliyanie strukturnykh parametrov na osobennosti elektronnoy struktury topologicheskikh poverkhnostnykh sostoyaniy MnBi2Te4

Experimental investigations of antiferromagnetic topological insulator MnBi2Te4 have shown that the energy gap in samples may vary in a wide range. Since the energy gap is a key parameter of this system when used in developing new functional electronic devices, the reason for variation of the MnBi2Te4 energy gap at the Dirac point and its possible interrelation with magnetic interactions are matters of great importance and call for thorough analysis. To elucidate factors influencing the energy gap, we analyzed the variation of the electronic structure of the given topological insulator with surface van der Waals gap. Calculation data have shown that the energy gap at such structure modifications may vary in a wide range from 80–88 meV to 4–5 meV because of an intense spatial redistribution of topological surface states between septuple-layer MnBi2Te4 blocks with oppositely directed Mn magnetic moments. Our results suggest that the spatial localization of topological surface states is a primary factor governing the value of the energy gap, this localization being strongly dependent on structure modifications on the crystal surface.

Magnetic properties of hematite revealed by an ab initio parameterized spin model

Hematite is a canted antiferromagnetic insulator, promising for applications in spintronics. Here we present ab initio calculations of the tensorial exchange interactions of hematite and use them to understand its magnetic properties by parametrizing a semiclassical Heisenberg spin model. Using atomistic spin dynamics simulations, we calculate the equilibrium properties and phase transitions of hematite, most notably the Morin transition. The computed isotropic and Dzyaloshinskii--Moriya interactions result in a N\'eel temperature and weak ferromagnetic canting angle that are in good agreement with experimental measurements. Our simulations show how dipole-dipole interactions act in a delicate balance with first and higher-order on-site anisotropies to determine the material's magnetic phase. Comparison with spin-Hall magnetoresistance measurements on a hematite single crystal reveals deviations of the critical behavior at low temperatures. Based on a mean-field model, we argue that these differences result from the quantum nature of the fluctuations that drive the phase transitions.

Giant nonlocal edge conduction in the axion insulator state of MnBi2Te4

The recently discovered antiferromagnetic (AFM) topological insulator (TI) MnBi2Te4 represents a versatile material platform for exploring exotic topological quantum phenomena in nanoscale devices. It has been proposed that even-septuple-layer (even-SL) MnBi2Te4 can host helical hinge currents with unique nonlocal behavior, but experimental confirmation is still lacking. In this work, we report transport studies of exfoliated MnBi2Te4 flakes with varied thicknesses down to the few-nanometer regime. We observe giant nonlocal transport signals in even-SL devices when the system is in the axion insulator state but vanishingly small nonlocal signal in the odd-SL devices at the same magnetic field range. In conjunction with theoretical calculations, we demonstrate that the nonlocal transport is via the helical edge currents mainly distributed at the hinges between the side and top/bottom surfaces. The helical edge currents in the axion insulator state may find unique applications in topological quantum devices.

Micromagnetic study of spin transport in easy-plane antiferromagnetic insulators

Magnon eigenmodes in easy-plane antiferromagnetic insulators are linearly polarized and are not expected to carry any net spin angular momentum. Motivated by recent nonlocal spin transport experiments in the easy-plane phase of hematite, we perform a series of micromagnetic simulations in a nonlocal geometry at finite temperatures. We show that by tuning an external magnetic field, we can control the magnon eigenmodes and the polarization of the spin transport signal in these systems. We argue that a coherent beating oscillation between two orthogonal linearly polarized magnon eigenmodes is the mechanism responsible for finite spin transport in easy-plane antiferromagnetic insulators. The sign of the detected spin signal is also naturally explained by the proposed coherent beating mechanism. Our finding opens a path for on-demand control of the spin signal in a large class of easy-plane antiferromagnetic insulators.

Topological driven linear magnetoresistance in Sb-doped MnBi2Te4

Linear magnetoresistance (LMR) is an attractive phenomenon that shows potential for uncovering novel physics and gauss sensor applications. Here we report a Fermi-level-sensitive LMR by doping Sb into antiferromagnetic topological insulator (TI) MnBi2Te4 crystals. The LMR is most remarkable when the Fermi level is close to the charge neutral point and the bulk carriers are largely suppressed. Our detailed analyses reveal that the slope of the LMR shows linear dependence on the inverse of carrier density. The results are quantitatively consistent with the quantum LMR model based on the surface state of a TI and thus reveal a transport signature of the topological surface state. Our work provides crucial insights into the understanding of the essential MR behavior and the surface state in MnBi2Te4.

Giant electrically tunable magnon transport anisotropy in a van der Waals antiferromagnetic insulator

Anisotropy is a manifestation of lowered symmetry in material systems that have profound fundamental and technological implications. For van der Waals magnets, the two-dimensional (2D) nature greatly enhances the effect of in-plane anisotropy. However, electrical manipulation of such anisotropy as well as demonstration of possible applications remains elusive. In particular, in-situ electrical modulation of anisotropy in spin transport, vital for spintronics applications, has yet to be achieved. Here, we realized giant electrically tunable anisotropy in the transport of second harmonic thermal magnons (SHM) in van der Waals anti-ferromagnetic insulator CrPS4 with the application of modest gate current. Theoretical modeling found that 2D anisotropic spin Seebeck effect is the key to the electrical tunability. Making use of such large and tunable anisotropy, we demonstrated multi-bit read-only memories (ROMs) where information is inscribed by the anisotropy of magnon transport in CrPS4. Our result unveils the potential of anisotropic van der Waals magnons for information storage and processing.

Magnetic transitions of hydrogenated H x CrO2 (x = 0–2) monolayer from a ferromagnetic half-metal to antiferromagnetic insulator

Two-dimensional (2D) transition metal oxide monolayers are currently attracting great interest in materials research due to their versatility and tunable electronic and magnetic properties. In this study, we report the prediction of magnetic phase changes in H x CrO2 (0 ⩽ x ⩽ 2) monolayer on the basis of first-principles calculations. As the H adsorption concentration x increases from 0 to 0.75, H x CrO2 monolayer transforms from a ferromagnetic (FM) half-metal to a small-gap FM insulator. When x = 1.00 and 1.25, it behaves as a bipolar antiferromagnetic (AFM) insulator, and eventually becomes an AFM insulator as x increases further up to 2.00. The results suggest that the magnetic properties of CrO2 monolayer can be effectively controlled by hydrogenation, and that H x CrO2 monolayers have the potential for realizing tunable 2D magnetic materials. Our results provide a comprehensive understanding of the hydrogenated 2D transition metal CrO2 and provide a research method that can be used as a reference for the hydrogenation of other similar 2D materials.

Intrinsic and extrinsic dopings in epitaxial films MnBi2Te4

The intrinsic antiferromagnetic topological insulator MnBi2Te4 and members of its family have been the subject of theoretical and experimental research, which has revealed the presence of a variety of defects and disorders that are crucial in determining the topological and magnetic properties. This also brings about challenges in realizing the quantum states like the quantum anomalous Hall and the axion insulator states. Here, utilizing cryogenic magnetoelectric transport and magnetic measurements, we systematically investigate the effects arising from intrinsic doping by antisite defects and extrinsic doping by Sb in MnBi2Te4 epitaxial films grown by molecular beam epitaxy. We demonstrate that the nonequilibrium condition in epitaxy allows a wide growth window for optimizing the crystalline quality and defect engineering. While the intrinsic antisite defects caused by the intermixing between Bi and Mn can be utilized to tune the Fermi level position as evidenced by a p-to-n conductivity transition, the extrinsic Sb-doping not only compensates for this doping effect but also modifies the magnetism and topology of the film, during which a topological phase transition is developed. Conflicting reports from the theoretical calculations and experimental measurements in bulk crystals versus epitaxial films are addressed, which highlights the intimate correlation between the magnetism and topology as well as the balance between the Fermi-level positioning and defect control. The present study provides an experimental support for the epitaxial growth of the intrinsic topological insulator and underlines that the topology, magnetism, and defect engineering should be revisited for enabling a steady and reliable film production.