We propose a realization of an antisymmetric spin-split band structure through magnetic phase transitions without spin-orbit coupling. It enables us to utilize for a variety of magnetic-order-driven cross-correlated and nonreciprocal transport phenomena as similar to those in the spin-orbit-coupling oriented systems. We unveil its general condition as an emergence of a bond-type magnetic toroidal multipole (polar tensor) in the triangular unit with the noncollinear 120$^{\circ}$-AFM structures. By using the concept of augmented multipoles, we systematically analyze the phenomena in terms of an effective multipole coupling. Our multipole description is ubiquitously applied to any trigonal and hexagonal structures including the triangular, kagome, and breathing kagome structures, which provides how to design and engineer materials with a giant antisymmetric spin splitting and its physical responses even without the spin-orbit coupling.
We present an algorithm for the numeric calculation of antiferromagnetic resonance frequencies for the non-collinear antiferromagnets of general type. This algorithm uses general exchange symmetry approach \cite{andrmar} and is applicable for description of low-energy dynamics of an arbitrary noncollinear spin structure in weak fields. Algorithm is implemented as a MatLab and C++ program codes, which are available for download. Program codes are tested against some representative analytically solvable cases.
Magnetoelectric and magnetoelastic phenomena correlated with a phase transition into noncollinear magnetic phase have been investigated for single crystals of CuFeO2 with a frustrated triangular lattice. CuFeO2 exhibits several long-wavelength magnetic structures related to the spin frustration, and it is found that finite electric polarization, namely inversion symmetry breaking, occurs with noncollinear but not at collinear magnetic phases. This result demonstrates that the noncollinear spin structure is a key role to induce electric polarization, and suggests that frustrated magnets which o…
Instability of the excitation spectrum of an ordered noncollinear Heisenberg antiferromagnet (AF) with respect to spontaneous two-magnon decays is investigated. We use a spin-1/2 AF on a triangular lattice as an example and examine the characteristic long- and short wave-length features of its zero-temperature spectrum within the 1/S-approximation. The kinematic conditions are shown to be crucial for the existence of decays and for overall properties of the spectrum. The XXZ and the J-J' generalizations of the model, as well as the role of higher-order corrections are discussed.
We present the detailed inelastic neutron scattering measurements of the noncollinear antiferromagnet Mn$_3$Ge. Time-of-flight and triple-axis spectroscopy experiments were conducted at the temperature of 6~K, well below the high magnetic ordering temperature of 370~K. The magnetic excitations have a 5-meV gap and display an anisotropic dispersive mode reaching $\simeq 90$~meV at the boundaries of the magnetic Brillouin zone. The spectrum at the zone center shows two additional excitations that demonstrate characteristics of both magnons and phonons. The \textit{ab initio} lattice-dynamics cal…
We study periodically driven insulating noncollinear stacked kagome antiferromagnets with a conventional symmetry-protected three-dimensional (3D) in-plane $120^\circ$ spin structure, with either positive or negative vector chirality. We show that the symmetry protection of the in-plane $120^\circ$ spin structure can be broken in the presence of an off-resonant circularly or linearly polarized electric field propagating parallel to the in-plane $120^\circ$ spin structure (say along the $x$ direction). Consequently, topological Floquet Weyl magnon nodes with opposite chirality are photoinduced …
We have measured antiferromagnetic resonance (AFMR) frequency-field dependences for aluminum-manganese garnet Mn$_{3}$Al$_{2}$Ge$_{3}$O$_{12}$ at frequencies from 1 to 125 GHz and at the fields up to 60 kOe. Three AFMR modes were observed for all orientations, their zero field gaps are about 40 and 70 GHz. Andreev-Marchenko hydrodynamic theory [Sov. Phys. Usp. 130, 39 (1980)] well describes experimental frequency-field dependences. We have observed hysteresis of resonance absorption as well as history dependence of resonance absorption near gap frequencies below 10 kOe in all three measured fi…
Antiferromagnetic spintronics is one of the leading candidates for next-generation electronics. Among abundant antiferromagnets, noncollinear antiferromagnets are promising for achieving practical applications due to coexisting ferromagnetic and antiferromagnetic merits. In this perspective, we briefly review the recent progress in the emerging noncollinear antiferromagnetic spintronics from fundamental physics to device applications. Current challenges and future research directions for this field are also discussed.
The antiferromagnet Mn$_5$Si$_3$ has recently attracted attention because a noncollinear spin arrangement has been shown to produce a topological anomalous Hall effect and an inverse magnetocaloric effect. Here we synthesize single crystals of Mn$_5$Si$_3$ using flux growth. We determine the phase diagram through magnetization and measure the magnetoresistance and the Hall effect. We find the collinear and noncollinear antiferromagnetic phases at low temperatures and, in addition, a third magnetic phase, in between the two antiferromagnetic phases which has ferromagnetic character. The latter …
Combining magnetism with band topology provides various novel phases that are otherwise impossible. Among several cases, noncollinear metallic antiferromagnets can reveal particularly rich topological physics due to their diverse magnetic ground states. However, there are only a few experimental studies due to the lack of suitable materials, especially with triangular lattice antiferromagnets. Here, we report that metallic triangular antiferromagnet Co1/3TaS2 exhibits a substantial anomalous Hall effect (AHE) related to its noncollinear magnetic order. Our first-principles calculations found t…
Motivated by the recently synthesized insulating nickelate Ni$_2$Mo$_3$O$_8$, which has been reported to have an unusual non-collinear magnetic order of Ni$^{2+}$ $S=1$ moments with a nontrivial angle between adjacent spins, we construct an effective spin-1 model on the honeycomb lattice, with the exchange parameters determined with the help of first principles electronic structure calculations. The resulting bilinear-biquadratic model, supplemented with the realistic crystal-field induced anisotropy, favors the collinear Néel state. We find that the crucial key to explaining the observed nonc…
By using the coupled cluster method, the numerical exact diagonalization method, and the numerical density matrix renormalization group method, we investigated the properties of the one-dimensional Heisenberg chain with alternating antiferromagnetic and ferromagnetic next nearest neighbor interactions. In the classical limit, the ground state is in the collinear Neel state if a<1/2, while for a>1/2, there is an noncollinear canted state. For the quantum case, we found that, although the classical Neel state is absent, the canted state exists if the frustration parameter a exceeds a critical po…
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…
A unified molecular field theory (MFT) is presented that applies to both collinear and planar noncollinear Heisenberg antiferromagnets (AFs) on the same footing. The spins in the system are assumed to be identical and crystallographically equivalent. This formulation allows calculations of the anisotropic magnetic susceptibility chi versus temperature T below the AF ordering temperature TN to be carried out for arbitrary Heisenberg exchange interactions J{ij} between arbitrary neighbors j of a given spin i without recourse to magnetic sublattices. The Weiss temperature theta_p in the Curie-Wei…
One of the main bottleneck issues for room-temperature antiferromagnetic spintronic devices is the small signal read-out owing to the limited anisotropic magnetoresistance in antiferromagnets. However, this could be overcome by either utilizing the Berry-curvature-induced anomalous Hall resistance in noncollinear antiferromagnets or establishing tunnel junction devices based on effective manipulation of antiferromagnetic spins. In this work, we demonstrate the giant piezoelectric strain control of the spin structure and the anomalous Hall resistance in a noncollinear antiferromagnetic metal - …
Noncollinear magnetic states in clusters are studied by using the single-band Hubbard Hamiltonian. The unrestricted Hartree-Fock (UHF) approximation is considered without imposing any symmetry constraints neither to the size or orientation of the local magnetic moments $<\vec S_l>$ nor to the local charge densities $<n_l>$. A variety of qualitatively different selfconsistent solutions is obtained as a function of cluster size, structure, number of valence electrons $ν$ and Coulomb interaction strength $U/t$. This includes inhomogeneous density distributions, paramagnetic solutions, magnetic so…
Collinear and noncollinear antiferromagnetic ordering in a highly frustrated decorated square kagomé lattice antiferromagnets of the nabokoite family
P.L. Kapitza Institute for Physical Problems, RAS（俄罗斯科学院P.L.卡皮察物理问题研究所）；National Research University “HSE”（国立研究型大学高等经济大学）；M.V. Lomonosov Moscow State University（莫斯科罗蒙诺索夫国立大学）；National University of Science and Technology “MISiS”（国立科技大学米西斯大学）
The kagome lattice antiferromagnets Mn$_3$X(= Sn, Ge) have a noncollinear 120$^\circ$ ordered ground state, which engenders a strong anomalous Hall response. It has been shown that this response is linked to the magnetic order and can be manipulated through it. Here we use a combination of strain and spin-transfer torques to control the magnetic order and hence switch deterministically between states of different chirality. Each of these chiral ground states has an anomalous Hall conductivity tensor in a different direction. Furthermore, we show that a similar manipulation of the strained samp…
Co4Ta2O9 exhibits a three-dimensional magnetic lattice based on the buckled honeycomb motif. It shows unusual magnetoelectric effects, including the sign change and non-linearity. These effects cannot be understood without the detailed knowledge of the magnetic structure. Herein, we report neutron diffraction and direction-dependent magnetic susceptibility measurements on Co4Ta2O9 single crystals. Below 20.3 K, we find a long-range antiferromagnetic order in the alternating buckled and flat honeycomb layers of Co2+ ions stacked along the c axis. Within experimental accuracy, the magnetic momen…
We report an unexpected magnetic-field-driven magnetic structure in the 5f-electron Shastry- Sutherland system U2Pd2In. This phase develops at low temperatures from a noncollinear antiferromagnetic ground state above the critical field of 25.8 T applied along the a-axis. All U moments have a net magnetic moment in the direction of the applied field, described by a ferromagnetic propagation vector qF = (0 0 0) and an antiferromagnetic component described by a propagation vector qAF = (0 0.30 1/2 ) due to a modulation in the direction perpendicular to the applied field. We conclude that this sur…
Direct imaging and control of Berry curvature in noncollinear antiferromagnetic single-crystal thin films
University of Wisconsin-Madison（威斯康星大学麦迪逊分校）；University of California, Irvine（加州大学尔湾分校）；University of Nebraska, Lincoln（内布拉斯加大学林肯分校）；University of Oxford（牛津大学）；University College London（伦敦大学学院）；STFC Rutherford Appleton Laboratory（英国科学与技术设施委员会鲁瑟福阿普尔顿实验室）
Temperature-invariant magneto-optical Kerr effect in a noncollinear antiferromagnet
University of California, Irvine（加州大学尔湾分校）；University of Wisconsin-Madison（威斯康星大学麦迪逊分校）；Irvine Materials Research Institute, University of California, Irvine（加州大学尔湾分校欧文材料研究所）；Colorado State University（科罗拉多州立大学）
Antiferromagnetic antiperovskites, of the form Mn$_3B$N ($B$ = Ni, Cu, Zn, Sn, Ir, and Pt), have shown an outstanding behavior in which, giant negative thermal expansion and chiral magnetic structures are intertwined. As such, aiming to shed light on the magnetostructural behavior, related to the magnetic ordering and structure of this type of materials, we studied by theoretical first-principles calculations the spin-phonon coupling in the Manganese-based antiperovskite Mn$_3$NiN, as a prototype in the Mn$_3B$N family. We found a strong spin-lattice coupling by means of the understanding of t…
High-resolution neutron diffraction determination of noncollinear antiferromagnetic order in the honeycomb magnetoelectric Fe$_{4}$Nb$_{2}$O$_{9}$
Institute for Basic Science (IBS)（韩国基础科学研究院）；Yonsei University（延世大学）；Chonnam National University（全南国立大学）；Center for Integrated Nanostructure Physics, Institute for Basic Science (IBS)（韩国基础科学研究院集成纳米物理中心）；Sungkyunkwan University（成均馆大学）；Rutgers University（罗格斯大学）
The Eu spins-7/2 in EuCo2P2 with the tetragonal ThCr2Si2-type structure have the prototypical noncollinear helical antiferromagnetic structure below the Neel temperature TN = 66.5 K as previously determined from single-crystal neutron diffraction measurements. The helix axis is along the c axis with the ordered moments aligned within the ab plane. Our recent formulation of molecular field theory (MFT) is found to quantitatively fit the anisotropic magnetic susceptibility of single-crystal EuCo2P2 at T < TN with a helix turn angle comparable to the neutron diffraction value. The experimental an…
A recently-developed molecular field theory (MFT) has been used to fit single-crystal magnetic susceptibility chi versus temperature T data below the respective antiferromagnetic ordering temperatures TN for a variety of collinear and coplanar noncollinear Heisenberg antiferromagnets. The spins in the system are assumed to interact by Heisenberg exchange and to be identical and crystallographically equivalent. The fitting parameters for chi(T) of collinear antiferromagnets are measurable quantities: the Weiss temperature theta_p in the Curie-Weiss law, TN, chi(TN), and the spin S. For coplanar…
We generalize the concept of the spin-momentum locking to magnonic systems and derive the formula to calculate the spin expectation value for one-magnon states of general two-body spin Hamiltonians. We give no-go conditions for magnon spin to be independent of momentum. As examples of the magnon spin-momentum locking, we analyze a one-dimensional antiferromagnet with the Néel order and two-dimensional kagome lattice antiferromagnets with the 120$^\circ$ structure. We find that the magnon spin depends on its momentum even when the Hamiltonian has the $z$-axis spin rotational symmetry, which can…
We theoretically study magnetic and topological properties of antiferromagnetic kagome spin systems in the presence of both in- and out-of-plane Dzyaloshinskii-Moriya interactions. In materials such as the iron jarosites, the in-plane interactions stabilize a canted noncollinear "umbrella" magnetic configuration with finite scalar spin chirality. We derive expressions for the canting angle, and use the resulting order as a starting point for a spin-wave analysis. We find topological magnon bands, characterized by non-zero Chern numbers. We calculate the magnon thermal Hall conductivity, and pr…
Investigation of materials that exhibit quantum phase transition provides valuable insights into fundamental problems in physics. We present neutron scattering under pressure in a triangular-lattice antiferromagnet which has a quantum disorder in the low-pressure phase and a noncollinear structure in the high-pressure phase. The neutron spectrum continuously evolves through the critical pressure; a single mode in the disordered state becomes soft with the pressure, and it splits into gapless and gapped modes in the ordered phase. Extended spin-wave theory reveals that the longitudinal and tran…
RbFe$^{2+}$Fe$^{3+}$F$_6$ is an example of a charge ordered antiferromagnet where iron sites, with differing valences, are structurally separated into two interpenetrating sublattices. The low temperature magnetically ordered Fe$^{2+}$ ($S$=2) and Fe$^{3+}$ ($S$=5/2) moments form a noncollinear orthogonal structure with the Fe$^{3+}$ site displaying a reduced static ordered moment. Neutron spectroscopy on single crystals finds two distinct spin wave branches with a dominant coupling along the Fe$^{3+}$ chain axis ($b$-axis). High resolution spectroscopic measurements find an intense energy and…
Elastic neutron scattering is used to study the spin correlations in the multiferroic $\rm Mn_{1-x}Fe_{x}WO_4$ with $x=0.035, 0.05$ and 0.10. The noncollinear, incommensurate (ICM) magnetic structure associated with the ferroelectric (FE) phase in pure $\rm MnWO_4$ is suppressed at $x=0.035$ and completely absent at $x=0.10$. The ICM spin order and FE phase can be restored by applying a magnetic field along the spin easy-axis. The low-$T$ commensurate magnetic structure extends in both H/T with increasing Fe concentration. The systematic evolution of the magnetic and electric properties indica…
We study a square-lattice spin-half Heisenberg model where frustration is introduced by competing nearest-neighbor bonds of different signs. We discuss the influence of quantum fluctuations on the nature of the zero-temperature phase transitions from phases with collinear magnetic order at small frustration to phases with noncollinear spiral order at large frustration. We use the coupled cluster method (CCM) for high orders of approximation (up to LSUB6) and the exact diagonalization of finite systems (up to 32 sites) to calculate ground-state properties. The role of quantum fluctuations is ex…
It is shown that the mechanism of order out of disorder is at work in the antisymmetric pyrochlore antiferromagnet. Quantum as well as thermal fluctuations break the continuous degeneracy of the classical ground state manifold and reduce its symmetry to $\mathbb{Z}_3 \times \mathbb{Z}_2$. The role of anisotropic symmetric exchange is also investigated and we conclude that this discrete like ordering is robust with respect to these second order like interactions. The antisymmetric pyrochlore antiferromagnet is therefore expected to order at low temperatures, whatever the symmetry type of its in…
We investigate the nature of phase transitions induced by Dzyaloshinskii-Moriya (DM) interactions on a classical pyrochlore antiferromagnet. For both symmetry-allowed antisymmetric exchange interactions, the macroscopic degeneracy due to geometrical frustration is relieved and a long-range magnetic order appears in the ground state. We find an Ising-like phase transition in the case of direct DM interaction which selects a doubly degenerate all-in all-out magnetic order. In the presence of indirect DM coupling, the magnet undergoes an XY-like phase transition into a state with broken Z6 symmet…
Our world is composed of various materials with different structures, where spin structures have been playing a pivotal role in spintronic devices of the contemporary information technology. Apart from conventional collinear spin materials such as collinear ferromagnets and collinear antiferromagnetically coupled materials, noncollinear spintronic materials have emerged as hot spots of research attention owing to exotic physical phenomena. In this Review, we firstly introduce two types noncollinear spin structures, i.e., the chiral spin structure that yields real-space Berry phases and the cop…
Novel effects induced by nonmagnetic impurities in frustrated magnets and quantum spin liquid represent a highly nontrivial and interesting problem. A theoretical proposal of extended modulated spin structures induced by doping of such magnets, distinct from the well-known skyrmions has attracted significant interest. Here, we demonstrate that nonmagnetic impurities can produce such extended spin structures in h-YMnO3, a triangular antiferromagnet with noncollinear magnetic order. Using inelastic neutron scattering (INS), we measured the full dynamical structure factor in Al-doped h-YMnO3 and …
We propose an efficient microscopic design procedure of electronic band structures having intrinsic spin and momentum dependences in spin-orbit-coupling free antiferromagnets. Our bottom-up design approach to creating desired spin-split and reshaped band structures could result in further findings of practical spin-orbit-coupling free materials exhibiting a giant spin-dependent and/or nonreciprocal transport, magneto-electric and elastic responses as a consequence of such band structures. We establish a systematic guideline to construct symmetric/antisymmetric spin-split and antisymmetrically …
CuCrO2 is a manifestation of a two-dimensional triangular antiferromagnet which exhibits an incommensurate noncollinear magnetic structure similar to a classical 120 degree ordering. Using the inelastic neutron scattering technique, direct evidence of a magnon-phonon coupling in CuCrO2 is revealed via the mixed magnon-phonon character of the excitation mode at 12.5 meV as well as a minimum at the zone boundary. A simple model Hamiltonian that incorporates an exchange striction type magnon-phonon coupling reproduces the observed features accurately. Also, continuum excitations originating from …
Motivated by the importance of non-collinear and non-coplanar magnetic phases in determining various electrical properties of magnetic materials, we investigate the phase diagrams of the extended Hubbard model on anisotropic triangular lattice. We make use of a mean-field scheme that treats collinear, non-collinear and non-coplanar phases on equal footing. In addition to the ferromagnetic and 120° antiferromagnetic phases, we find the four-sublattice flux, the 3Q non-coplanar and the non-collinear charge-ordered states to be stable at specific values of filling fraction $n$. Inter-site Coulomb…
Terahertz time-domain spectroscopy was performed to directly probe the low-energy (1-5 meV) electrodynamics of triangular lattice antiferromagnets CuFe1-xGaxO2 (x = 0.00, 0.01, and 0.035). We discovered an electromagnon (electric-field-active magnon) excitation at 2.3 meV in the paraelectric up-up-down-down collinear magnetic phase, while this electromagnon vanishes in the ferroelectric helimagnetic phase. Anti-correlation with noncollinear magnetism excludes the exchange-striction mechanism as the origin of dynamical magnetoelectric coupling, and hence evidences the observation of spin-orbit …
Dielectric responses have been investigated on the triangular-lattice antiferromagnet CuFeO2 and its site-diluted analogs CuFe1-xAlxO2 (x=0.01 and 0.02) with and without application of magnetic field. We have found a ferroelectric behavior at zero magnetic field for x=0.02. At any doping level, the onset field of the ferroelectricity always coincides with that of the noncollinear magnetic structure while the transition field dramatically decreases to zero field with Al doping. The results imply the further possibility of producing the ferroelectricity by modifying the frustrated spin structure…
The theory of exchange symmetry of spin ordered states is extended to the case of high magnetic field. Low frequency spin dynamics equation for quasi-goldstone mode is derived for two cases of collinear and noncollinear antiferromagnets.
We report our theoretical results on spin conductivity in antiferromagnets by focusing on the role of the magnetic toroidal quadrupole (MTQ) in electron systems. The MTQ is characterized as a time-reversal-odd rank-2 polar tensor degree of freedom in electrons, which is distinct from conventional rank-1 magnetic and magnetic toroidal dipoles. Based on a microscopic $sd$ model analysis for a tetragonal system under both collinear and noncollinear antiferromagnetic orderings, we clarify that the MTQ becomes a source of an extrinsic spin conductivity even with neither a uniform magnetization nor …
Elementary quasiparticles in solids such as phonons and magnons occasionally have nontrivial interactions between them, as well as among themselves. As a result, their energy eigenvalues are renormalized, the quasiparticles spontaneously decay into a multi-particle continuum state, or they are hybridized with each other when their energies are close. As discussed in this review, such anomalous features can appear dominantly in quantum magnets but are not, a priori, negligible for magnetic systems with larger spin values and noncollinear magnetic structures. We review the unconventional magneti…
Breakdown of the conventional spin-wave dynamics and its double-constraint modification in the spin-$\mathbf{\frac{1}{2}}$ triangular-prism Heisenberg antiferromagnet
Quantum phase transitions in the two-dimensional Kugel-Khomski model on a square lattice are studied using the plaquette mean field theory and the entanglement renormalization ansatz. When $3z^2-r^2$ orbitals are favored by the crystal field and Hund's exchange is finite, both methods give a noncollinear exotic magnetic order which consists of four sublattices with mutually orthogonal nearest neighbor and antiferromagnetic second neighbor spins. We derive effective frustrated spin model with second and third neighbor spin interactions which stabilize this phase and follow from spin-orbital qua…
We have used resonant x-ray diffraction to develop a detailed description of antiferromagnetic ordering in epitaxial superlattices based on two-unit-cell thick layers of the strongly correlated metal LaNiO3. We also report reference experiments on thin films of PrNiO3 and NdNiO3. The resulting data indicate a spiral state whose polarization plane can be controlled by adjusting the Ni d-orbital occupation via two independent mechanisms: epitaxial strain and quantum confinement of the valence electrons. The data are discussed in the light of recent theoretical predictions.
Neutron inelastic scattering and diffraction techniques have been used to study the MnV2O4 spinel system. Our measurements show the existence of two transitions to long-range ordered ferrimagnetic states; the first collinear and the second noncollinear. The lower temperature transition, characterized by development of antiferromagnetic components in the basal plane, is accompanied by a tetragonal distortion and the appearance of a gap in the magnetic excitation spectrum. The low-temperature noncollinear magnetic structure has been definitively resolved. Taken together, the crystal and magnetic…
