Time-reversal symmetry breaking is the basic physics concept underpinning many magnetic topological phenomena such as the anomalous Hall effect (AHE) and its quantized variant. The AHE has been primarily accompanied by a ferromagnetic dipole moment, which hinders the topological quantum states and limits data density in memory devices, or by a delicate noncollinear magnetic order with strong spin decoherence, both limiting their applicability. A potential breakthrough is the recent theoretical prediction of the AHE arising from collinear antiferromagnetism in an anisotropic crystal environment. This new mechanism does not require magnetic dipolar or noncollinear fields. However, it has not been experimentally observed to date. Here we demonstrate this unconventional mechanism by measuring the AHE in an epilayer of a rutile collinear antiferromagnet RuO$_2$. The observed anomalous Hall conductivity is large, exceeding 300 S/cm, and is in agreement with the Berry phase topological transport contribution. Our results open a new unexplored chapter of time-reversal symmetry breaking phenomena in the abundant class of collinear antiferromagnetic materials.
In a collinear antiferromagnet with easy-axis anisotropy, symmetry guarantees that the spin wave modes are doubly degenerate. The two modes carry opposite spin angular momentum and exhibit opposite chirality. Using a honeycomb antiferromagnet in the presence of the Dzyaloshinskii-Moriya interaction, we show that a longitudinal temperature gradient can drive the two modes to opposite transverse directions, realizing a spin Nernst effect of magnons with vanishing thermal Hall current. We find that magnons around the Γ-point and the K-point contribute oppositely to the transverse spin transport, …
We obtain the non-collinear ground states of a triangular-lattice antiferromagnet with exchange interactions up to third nearest neighbors as a function of the single-ion anisotropy $D$. At a critical value of $D$, the collinear $\uudd $ phase transforms into a complex non-collinear phase with odd-order harmonics of the fundamental ordering wavevector $\vQ $. The observed elastic peaks at $2π\vx -\vQ $ in both Al- and Ga- doped CuFeO$_2$ are explained by a "scalene" distortion of the triangular lattice produced by the repulsion of neighboring oxygen atoms.
We report on magneto-optical studies of the quasi-two-dimensional van der Waals antiferromagnet FePS$_3$. Our measurements reveal an excitation that closely resembles the antiferromagnetic resonance mode typical of easy-axis antiferromagnets, nevertheless, it displays an unusual, four-times larger Zeeman splitting in an applied magnetic field. We identify this excitation with an $|S_z|=4$ multipolar magnon -- a single-ion 4-magnon bound state -- that corresponds to a full reversal of a single magnetic moment of the Fe$^{2+}$ ion. We argue that condensation of multipolar magnons in large-spin m…
The correct stacking of hexagonal layers is used to obtain accurate estimates for the exchange and anisotropy parameters of the geometrically-frustrated antiferromagnet CuFeO$_2$. Those parameters are highly constrained by the stability of a collinear metamagnetic phase between fields of 13.5 and 20 T. Constrained fits of the spin-wave frequencies of the collinear $\uudd $ phase below 7 T are used to identify the magnetic unit cell of the metamagnetic $\uuudd $ phase, which contains two hexagonal layers and 10 Fe$^{3+}$ spins.
Non-collinear chiral antiferromagnets like Mn3Sn and Mn3Ge are known to show gigantic anomalous Hall response depending on the orientation of their inverse chiral magnetic order of Mn atoms in Kagome layers. Here we study the stability of such magnetic order in the absence of external magnetic fields on the basis of stochastic Landau-Lifshitz-Gilbert equation for a simplified two-dimensional model of these materials. We find that even without external magnetic fields, the ordered state is, once formed, highly stable against thermal fluctuations. Moreover, we show that if Mn spins are well conf…
We resolve the domain-wall structure of the model antiferromagnet $\text{Cr}_2\text{O}_3$ using nanoscale scanning diamond magnetometry and second-harmonic-generation microscopy. We find that the 180$^\circ$ domain walls are predominantly Bloch-like, and can co-exist with Néel walls in crystals with significant in-plane anisotropy. In the latter case, Néel walls that run perpendicular to a magnetic easy axis acquire a well-defined chirality. We further report quantitative measurement of the domain-wall width and surface magnetization. Our results provide fundamental input and an experimental m…
A systematic framework to investigate spin dynamics in non-collinear antiferromagnet is proposed. Taking Mn$_3$Sn as a representative example, we derive an effective low energy model based on the multipole expansion of the magnetic structure, and investigate the uniform precession and the domain wall dynamics. We show that the solution for the effective model accurately reproduces the numerical calculation of the Landau-Lifshitz-Gilbert equations. Our results indicate that Mn$_3$Sn has preferable properties for applications to a racetrack memory and a spin torque oscillator, and thus, is a pro…
Predictions of the anisotropic magnetic susceptibility chi below the antiferromagnetic (AFM) ordering temperatures TN of local moment Heisenberg AFMs have been made previously using molecular field theory (MFT) but are very limited in their applicability. Here a MFT calculation of chi(T<=TN) is presented for a wide variety of collinear and noncollinear Heisenberg AFMs containing identical crystallographically equivalent spins without recourse to magnetic sublattices. The results are expressed in terms of directly measurable experimental parameters and are fitted with no adjustable parameters t…
The anomalous Hall effect (AHE), which in long-range ordered ferromagnets appears as a voltage transverse to the current and usually is proportional to the magnetization, often is believed to be of negligible size in antiferromagnets due to their low uniform magnetization. However, recent experiments and theory have demonstrated that certain antiferromagnets with a non-collinear arrangement of magnetic moments exhibit a sizeable spontaneous AHE at zero field due to a non-vanishing Berry curvature arising from the quantum mechanical phase of the electron's wave functions. Here we show that anti…
Electric susceptibility of antiferromagnetic multiferroics with cycloidal spin order at magnetoelectric effect associated with collinear component of spins
We report a comprehensive study of magnetic properties of Ni3TeO6. The system crystallizes in a noncentrosymmetric rhombohedral lattice, space group R3. There are three differently coordinated Ni atoms in the unit cell. Two of them form an almost planar honeycomb lattice, while the third one is placed between the layers. Magnetization and specific heat measurements revealed a single magnetic ordering at TN = 52 K. Below TN the susceptibility with the magnetic field parallel to the c-axis drops towards zero while the perpendicular susceptibility remains constant, a characteristic of antiferroma…
Electrical detection of the 180 deg spin reversal, which is the basis of the operation of ferromagnetic memories, is among the outstanding challenges in the research of antiferromagnetic spintronics. Analogous effects to the ferromagnetic giant or tunneling magnetoresistance have not yet been realized in antiferromagnetic multilayers. Anomalous Hall effect (AHE), which has been recently employed for spin reversal detection in non-collinear antiferromagnets, is limited to materials that crystalize in ferromagnetic symmetry groups. Here we demonstrate electrical detection of the 180 deg Néel vec…
Spin photogalvanic effect (SPGE) is an efficient method to generate a spin current by photoexcitation in a contactless and ultra-fast way. In two-dimensional (2D) collinear antiferromagnetic (AFM) materials that preserve the combined time-reversal (T) and inversion (I) symmetry (i.e., TI symmetry), we find that the photogalvanic currents in two magnetic sublattices carry different kinds of spins and propagate in opposite direction if the spin-orbit coupling is negligible, resulting in a pure spin current without net charge current. Based on the first-principles calculations, we show that two e…
In the spirit of searching for Gd-based, frustrated, rare earth magnets, we have found antiferomagnetism (AF) in GdPtPb which crystallizes in the ZrNiAl-type structure that has a distorted Kagomé lattice of Gd-triangles. Single crystals were grown and investigated using structural, magnetic, transport and thermodynamic measurements. GdPtPb orders antiferromagnetically at 15.5 K arguably with a planar, non-collinear structure. The high temperature magnetic susceptibility data reveal an "anti-frustration" behavior having a frustration parameter, $|f|$ = $|Θ|$/ $T_N$ = 0.25, which can be explaine…
Electrical spin-current generation is among the core phenomena driving the field of spintronics. Using {\em ab initio} calculations we show that a room-temperature metallic collinear antiferromagnet RuO$_2$ allows for highly efficient spin-current generation, arising from anisotropically-split bands with conserved up and down spins along the Néel vector axis. The zero net moment antiferromagnet acts as an electrical spin-splitter with a 34$^\circ$ propagation angle between spin-up and spin-down currents. Correspondingly, the spin-conductivity is a factor of three larger than the record value f…
By combining two independent approaches, inelastic neutron scattering measurements and density functional theory calculations, we study the spin-waves in the high-temperature collinear antiferromagnetic phase (AFM2) of Mn$_5$Si$_3$. We obtain its magnetic ground-state properties and electronic structure. This study allowed us to determine the dominant magnetic exchange interactions and magnetocrystalline anisotropy in the AFM2 phase of Mn$_5$Si$_3$. Moreover, the evolution of the spin excitation spectrum is investigated under the influence of an external magnetic field perpendicular to the ani…
Magnetic annealing of the collinear antiferromagnet PdMn with excess Pd produces strongly pinned magnetic moments in the annealing field direction. This behaviour can be understood with the help of the magnetic-field-biased diffusion model. Here, the magnetic field creates an energy difference between the two possible occupations of the antiferromagnetic Mn-sublattices by the Pd-excess atoms. This, mediated by diffusion, leads to an imbalance in the amount of the Pd-excess atoms in these sublattices and, subsequently, to an imbalance in the total magnetization of the sublattices. We investigat…
Magnetic frustration in three dimensions (3D) manifests itself in the spin-$\frac12$ insulator Li$_2$CuW$_2$O$_8$. Density-functional band-structure calculations reveal a peculiar spin lattice built of triangular planes with frustrated interplane couplings. The saturation field of 29 T contrasts with the susceptibility maximum at 8.5 K and a relatively low Néel temperature $T_N\simeq 3.9$ K. Magnetic order below $T_N$ is collinear with the propagation vector $(0,\frac12,0)$ and an ordered moment of 0.65(4) $μ_B$ according to neutron diffraction data. This reduced ordered moment together with t…
Previous studies on the anomalous Hall effect in coplanar non-collinear antiferromagnets are revisited and extended to magneto-optic properties, namely magneto-optic Kerr effect (MOKE) and X-ray magnetic dichroism (XMCD). Starting from group-theoretical considerations the shape of the frequency-dependent conductivity tensor for various actual and hypothetical spin configurations in cubic and hexagonal Mn$_3X$ compounds is determined. Calculated MOKE and X-ray dichroism spectra are used to confirm these findings and to give estimates of the size of the effects. For Mn$_3$IrPt and Mn$_3$PtRh all…
Using symmetry arguments and a tight-binding model, we show that for layered collinear anti- ferromagnets, magneto-optic effects can be generated and manipulated by controlling crystal symmetries through a gate voltage. This provides a promising route for electric field manipulation of the magneto-optic effects without modifying the underlying magnetic structure. We further demonstrate the gate control of magneto-optic Kerr effect (MOKE) in bilayer MnPSe3 using first-principles calculations. The field-induced inversion symmetry breaking effect leads to gate-controllable MOKE whose direction of…
Antiferromagnets offer spintronic device characteristics unparalleled in ferromagnets owing to their lack of stray fields, THz spin dynamics, and rich materials landscape. Microscopic imaging of aniferromagnetic domains is one of the key prerequisites for understading physical principles of the device operation. However, adapting common magnetometry techniques to the dipolar-field-free antiferromagnets has been a major challenge. Here we demonstrate in a collinear antiferromagnet a thermoelectric detection method by combining the magneto-Seebeck effect with local heat gradients generated by sc…
The magnetic anisotropy of antiferromagnets plays a crucial role in stabilising the magnetisation of many spintronic devices. In non-collinear antiferromagnets such as IrMn the symmetry and temperature dependence of the effective anisotropy are poorly understood. Theoretical and experimental calculations of the effective anisotropy constant for IrMn differ by two orders of magnitude, while the symmetry has been calculated as uniaxial in contradiction to the assumed relationship between crystallographic symmetry and temperature dependence of the anisotropy from the Callen-Callen law. In this le…
We study the magnetic properties of small Mn ring shaped clusters on a Pt(111) surface in the framework of density functional theory. We find that the Mn atoms possess large magnetic moments, of the order of 4uB/atom, and have dominating antiferromagnetic interatomic exchange interactions. A quantum confinement effect within the ring like clusters was found, indicating that even very small clusters can be seen as quantum corrals. The antiferromagnetic exchange couplings lead to collinear magnetic arrangements in simple corrals, as well as complex non-collinear ordering, as vortex-like structur…
We report on Cr doping effect in Mn3Sn polycrystalline films with both uniform and modulation doping. It is found that Cr doping with low concentration does not cause notable changes to the structural and magnetic properties of Mn3Sn, but it significantly enhances the anomalous Hall conductivity, particularly for modulation-doped samples at low temperature. A Hall conductivity as high as 184.8 Ω-1 cm-1 is obtained for modulation-doped samples at 50 K, in a sharp contrast to vanishingly small values for undoped samples at the same temperature. We attribute the enhancement to the change of Fermi…
Although a cubic phase of Mn$_3$Ga with an antiferromagnetic order has been theoretically predicted, it has not been experimentally verified in a bulk or film form. Here, we report the structural, magnetic, and electrical properties of antiferromagnetic cubic Mn$_3$Ga (C-Mn$_3$Ga) thin films, in comparison with ferrimagnetic tetragonal Mn$_3$Ga (T-Mn3Ga). The structural analyses reveal that C-Mn$_3$Ga is hetero-epitaxially grown on MgO substrate with the Cu$_3$Au-type cubic structure, which transforms to T-Mn$_3$Ga as the RF sputtering power increases. The magnetic and magnetotransport data sh…
We set forth the structural and magnetic properties of the frustrated spin-$5/2$ triangle lattice antiferromagnet Na$_3$Fe(PO$_4$)$_2$ examined via x-ray diffraction, magnetization, heat capacity, and neutron diffraction measurements on the polycrystalline sample. No structural distortion was detected from the temperature-dependant x-ray diffraction down to 12.5 K, except a systematic lattice contraction. The magnetic susceptibility at high temperatures agrees well with the high-temperature series expansion for a spin-$5/2$ isotropic triangular lattice antiferromagnet with an average exchange …
The non-collinear antiferromagnetic (AFM) structure makes Mn3Sn exhibit exotic properties. At present, it has been found that both the hydrostatic pressure and the strain introduced by interstitial N atoms have a great influence on this magnetic structure. Here, the effect of the residual strain (RS) on it is investigated. AC and DC magnetic measurement results suggest that Mn3Sn without RS has the non-collinear AFM structure only in the temperature range of 285 K to 400 K; while Mn3Sn with RS has a non-coplanar AFM structure in the entire temperature range from 5 K to 400 K. Both anomalous Ha…
The anomalous Hall effect is investigated theoretically by means of density functional calculations for the non-collinear antiferromagnetic order of the hexagonal compounds Mn$_3$Ge and Mn$_3$Sn using various planar triangular magnetic configurations as well as unexpected non-planar configurations. The former give rise to anomalous Hall conductivities (AHC) that are found to be extremely anisotropic. For the planar cases the AHC is connected with Weyl-points in the energy-band structure, which are described in detail. If this case were observable in Mn$_3$Ge, a large AHC of about 900 S/cm shou…
We report on the ultrafast dynamics of magnetic order in a single crystal of CuO at a temperature of 207 K in response to strong optical excitation using femtosecond resonant x-ray diffraction. In the experiment, a femtosecond laser pulse induces a sudden, nonequilibrium increase in magnetic disorder. After a short delay ranging from 400 fs to 2 ps, we observe changes in the relative intensity of the magnetic ordering diffraction peaks that indicate a shift from a collinear commensurate phase to a spiral incommensurate phase. These results indicate that the ultimate speed for this antiferromag…
We investigate topological features of electronic structures which produce large anomalous Hall effect in the non-collinear antiferromagnetic metallic states of anti-perovskite manganese nitrides by first-principles calculations. We first predict the stable magnetic structures of these compounds to be non-collinear antiferromagnetic structures characterized by either $T_{1g}$ or $T_{2g}$ irreducible representation by evaluating the total energy for all of the magnetic structures classified according to the symmetry and multipole moments. The topology analysis is next performed for the Wannier …
We report a combined study of imaging the antiferromagnetic (AFM) spin structure and measuring the spin Hall magnetoresistance (SMR) in epitaxial thin films of the insulating non-collinear antiferromagnet SmFeO$_3$. X-ray magnetic linear dichroism photoemission electron microscopy measurements reveal that the AFM spins of the SmFeO$_3$(110) align in the plane of the film. Angularly dependent magnetoresistance measurements show that SmFeO$_3$/Ta bilayers exhibit a positive SMR, in contrast to the negative SMR expected in previously studied collinear AFMs. The SMR amplitude increases linearly wi…
Current-induced spin torques provide efficient data writing approaches for magnetic memories. Recently, the spin splitting torque (SST) was theoretically predicted (R. González-Hernández et al. Phys. Rev. Lett. 126, 127701 (2021)), which combines advantages of conventional spin transfer torque (STT) and spin-orbit torque (SOT) as well as enables controllable spin polarization. Here we provide the experimental evidence of SST in collinear antiferromagnet RuO2 films. The spin current direction is found to be correlated to the crystal orientation of RuO2 and the spin polarization direction is dep…
We provide a complete and systematic first-principles study of the thermodynamic stability, structural parameters, and magnetic properties of the T1 non-collinear antiferromagnetic L1$_2$-IrMn$_3$ surface and L1$_2$-IrMn$_3$/Fe heterostructure. Furthermore, we investigate the exchange-bias effect in the heterostructure and describe its previously unknown complex magnetic coupling at the interface. We consider four atomic configurations and four magnetic arrangements, finding two stable terminations for the surface and for the heterostructure, which are in good agreement with experimental HR-TE…
We report the anomalous Hall effect (AHE) in antiperovskite Mn$_{3}$NiN with substantial doping of Cu on the Ni site (i.e. Mn$_{3}$Ni$_{1-x}$Cu$_{x}$N), which stabilizes a noncollinear antiferromagnetic (AFM) order compatible with the AHE. Observed on both sintered polycrystalline pieces and single crystalline films, the AHE does not scale with the net magnetization, contrary to the conventional ferromagnetic case. The existence of the AHE is explained through symmetry analysis based on the $Γ_{\rm 4g}$ AFM order in Cu doped Mn$_{3}$NiN. DFT calculations of the intrinsic contribution to the AH…
The spin chirality, created by magnetic atoms, has been comprehensively understood to generate and control the magneto-optical effects. In comparison, the role of the crystal chirality that relates to nonmagnetic atoms has received much less attention. Here, we theoretically discover the crystal chirality magneto-optical (CCMO) effects, which depend on the chirality of crystal structures that originates from the rearrangement of nonmagnetic atoms. We show that the CCMO effects exist in many collinear antiferromagnets, such as RuO$_{2}$ and CoNb$_{3}$S$_{6}$, which has a local and global crysta…
The anomalous Hall effect (AHE) is a well-known fundamental property of ferromagnetic metals, commonly associated with the presence of a net magnetization. Recently, an AHE has been discovered in non-collinear antiferromagnetic (AFM) metals. Driven by non-vanishing Berry curvature of AFM materials with certain magnetic space group symmetry, anomalous Hall conductivity (AHC) is very sensitive to the specific type of magnetic ordering. Here, we investigate the appearance of AHC in antiperovskite GaNMn$_{3}$ as a representative of broader materials family ANMn$_{3}$ (A is a main group element), w…
The spin-Hall effect describes the interconversion of charge currents and spin currents, enabling highly efficient manipulation of magnetization for spintronics. Symmetry conditions generally restrict polarizations of these spin currents to be orthogonal to both the charge and spin flows. Spin polarizations can deviate from such direction in nonmagnetic materials only when the crystalline symmetry is reduced11. Here we experimentally show control of the spin polarization direction by using a non-collinear antiferromagnet Mn$_{3}$GaN, in which the triangular spin structure creates a low magneti…
The spin-splitter effect is theoretically predicted to generate an unconventional spin current with $\mathit{x}$- and $\mathit{z}$- spin polarization via the spin-split band in antiferromagnets. The generated torque, namely spin-splitter torque, is effective for the manipulation of magnetization in an adjacent magnetic layer without an external magnetic field for spintronic devices such as MRAM. Here, we study the generation of torque in collinear antiferromagnetic RuO$_2$ with (100), (101), and (001) crystal planes. Next we find all $\mathit{x}$-, $\mathit{y}$-, and $\mathit{z}$-polarized spi…
Local multiferroic ordering at room temperature in collinear magnetoelectric antiferromagnets induced by flexo-Zeeman coupling
Helmholtz-Zentrum Dresden-Rossendorf e.V.（德累斯顿-罗森多夫亥姆霍兹中心）；Faculty of Physics of Dresden University of Technology（德累斯顿工业大学物理学院）；Helmholtz-Zentrum Berlin für Materialien und Energie（柏林亥姆霍兹材料与能源中心）；Department of Applied Physics, KTH Royal Institute of Technology（瑞典皇家理工学院应用物理系）
