Complex Spin Structures and Origin of the Magneto-Electric Coupling in YMn2O5
J. -H. Kim, S. -H. Lee, S. I. Park, M. Kenzelmann, J. Schefer, J. -H. Chung, C. F. Majkrzak, M. Takeda, S. Wakimoto, S. Y. Park, S-W. Cheong, M. Matsuda, H. Kim… 展开作者
J. -H. Kim, S. -H. Lee, S. I. Park, M. Kenzelmann, J. Schefer, J. -H. Chung, C. F. Majkrzak, M. Takeda, S. Wakimoto, S. Y. Park, S-W. Cheong, M. Matsuda, H. Kimura, Y. Noda, K. Kakurai
By combining neutron four-circle diffraction and polarized neutron diffraction techniques we have determined the complex spin structures of a multiferroic, YMn2O5, that exhibits two ferroelectric phases at low temperatures. The obtained magnetic structure has spiral components in both the low temperature ferroelectric phases that are magnetically commensurate and incommensurate, respectively. Among proposed microscopic theories for the magneto-electric coupling, our results are consistent with both the spin-current model that requires a magnetic transverse (cycloidal) spiral structure in order to induce a spontaneous electric polarization and the magneto-restriction model. Our results also explain why the electric polarization changes at the commensurate-to-incommensurate phase transition.
Magneto-electric multipoles, which are odd under both space-inversion $\cal I$ and time-reversal $\cal T$ symmetries, are fundamental in understanding and characterizing magneto-electric materials. However, the detection of these magneto-electric multipoles is often not straightforward as they remain "hidden" in conventional experiments in part since many magneto-electrics exhibit combined $\cal IT$ symmetry. In the present work, we show that the anti-symmetric Compton profile is a unique signature for all the magneto-electric multipoles, since the asymmetric magnetization density of the magne…
The present paper proposes the direct calculation of the microscopic contributions to the magneto-electric coupling, using ab initio methods. The electrostrictive and the Dzyaloshinskii-Moriya contributions were evaluated individually. For this purpose a specific method was designed, combining DFT calculations and embedded fragments, explicitely correlated, quantum chemical calculations. This method allowed us to calculate the evolution of the magnetic couplings as a function of an applied electric field. We found that in $\rm YMnO_3$ the Dzyaloshinskii-Moriya contribution to the magneto-elect…
Two prominent magnetoelectrics MnWO$_4$ and CuO possess low-temperature commensurate paraelectric magnetically ordered phase. Here using Monte Carlo simulations we show that the walls between the domains of this phase are ferroelectric with the same electric polarization direction and value as that in the magnetoelectric phases of these compounds. We also suggest that experimental observation of electric polarization of domain walls in MnWO$_4$ should help to determine the macroscopic interactions responsible for its magnetoelectric properties.
We present a phenomenological scheme to study the size-dependent electric voltage-controlled magnetic anisotropy in ferromagnetic (FM)/ferroelectric (FE) heterostructures. The FM layers are either metallic Fe(001), Ni(001), Co(0001), or half-metallic (La, Sr)MnO3 films. Two magnetoelectric mechanisms, i.e., interface-charge and strain-mediated couplings, are considered. We show that the interface-charge mediated coupling is the main mechanism for the magnetoelectic coupling when the FM film thickness is below a certain transition thickness dtr while the strain-mediated coupling dominates above…
Our results describe an unprecedented example of change in the mechanism of magnetically-induced electric polarization from spin current to spin-dependent p-d hybridization model. We have followed the evolution of the magnetic structures of (ND4)2[FeCl5 D2O] compound using single crystal neutron diffraction under external magnetic field. The spin arrangements change from incommensurate cycloidal to commensurate distorted-cycloidal and finally to quasi-collinear. The determination of the magnetic structures allows us to explain the observed electric polarization in the different ferroelectric p…
A layered iron oxide \rfeo ($R$: rare-earth elements) is an exotic dielectric material with charge-order (CO) driven electric polarization and magnetoelectric effect caused by spin-charge coupling. In this paper, a theory of electronic structure and dielectric property in \rfeo is presented. Charge frustration in paired-triangular lattices allows a charge imbalance without inversion symmetry. Spin frustration induces reinforcement of this polar CO by a magnetic ordering. We also analyze an orbital model for the Fe ion which does not show a conventional long-range order.
We report on the exchange bias between antiferromagnetic and ferroelectric hexagonal YMnO3 epitaxial thin films sandwiched between a metallic electrode (Pt) and a soft ferromagnetic layer (Py). Anisotropic magnetoresistance measurements are performed to monitor the presence of an exchange bias field. When the heteroestructure is biased by an electric field, it turns out that the exchange bias field is suppressed. We discuss the dependence of the observed effect on the amplitude and polarity of the electric field. Particular attention is devoted to the role of current leakage across the ferroel…
Synthesis and extensive structural, pyroelectric, magnetic, dielectric and magneto-electric characterizations are reported for polycrystalline Co4Nb2O9 towards unraveling the multiferroic state especially in reference to the magnetic spin flop transition. Magnetic measurements confirm the Co4Nb2O9 becomes antiferromagnetic (AFM) at around 28 K but no clear evidence for spin-flop effect was found. Associated with the magnetic phase transition, a sharp peak in pyroelectric current indicates the appearance of the strong magneto-electric coupling below Neel temperature (TN) with a large coupling c…
We report remarkable multiferroic effects in polycrystalline Bi2Fe4O9. High-resolution X-ray diffraction shows that this compound has orthorhombic structure. Magnetic measurements confirm an antiferromagnetic transition around 260 K. A pronounced inverse S-shape anomaly in the loss tangent of dielectric measurement is observed near the Neel temperature. This feature shifts with the application of magnetic field. These anomalies are indicative of substantial coupling between the electric and magnetic orders in this compound.
We have determined the terahertz spectrum of the chiral langasite Ba$_3$NbFe$_3$Si$_2$O$_{14}$ by means of synchrotron-radiation measurements. Two excitations are revealed that are shown to have a different nature. The first one, purely magnetic, is observed at low temperature in the magnetically ordered phase and is assigned to a magnon. The second one persits far into the paramagnetic phase and exhibits both an electric and a magnetic activity at slightly different energies. This magnetoelectric excitation is interpreted in terms of atomic rotations and requires a helical electric polarizati…
Low energy excitations in the multiferroic material TbMnO3 have been investigated by Raman spectroscopy. Our observations reveal the existence of two peaks at 30 cm-1 and 60 cm-1. They are observed in the cycloidal phase below the Curie temperature but not in the sinusoidal phase, suggesting their magnetoelectric origin. While the peak energies coincide with the frequencies of electromagnons measured previously by transmission spectroscopy, they show surprisingly different selection rules, with the 30 cm-1 excitation enhanced by the electric field of light along the spontaneous polarization. T…
Magneto-dielectric spectra of La0.95Ca0.05CoO3 covering the crossover of spin states reveals strong coupling of its spin and dipolar degrees of freedom. Signature of spin-state transition at 30K clearly manifests in magnetization, supported by Co L_3,2-edge XAS data on the doped-specimen as consistent with its suppressed T_SST vs. ~150K for pure LaCoO3. Dispersive activation-step Δε'(T_ω)~O(10^2) and relaxation-peak ε"(T_ω) reflect the allied influence of coexistent spin-states on the dielectric character. Dipolar relaxation in the LS regime below T_SST is partly segmental (VFT kinetics) featu…
Exploring possible magnetic monopoles-induced magneto-electricity in spin ices
University of Geneva（日内瓦大学）；Institut Néel, CNRS and Université Grenoble Alpes（内勒研究所，法国国家科学研究中心与格勒诺布尔阿尔卑斯大学）；ICMMO, Université Paris-Saclay, CNRS（物质化学与分子和超分子研究所，巴黎萨克雷大学，法国国家科学研究中心）
With a combined ab initio density functional and model Hamiltonian approach we establish that in the recently discovered multiferroic phase of the manganite Sr$_{1/2}$Ba$_{1/2}$MnO$_{3}$ the polar distortion of Mn and O ions is stabilized via enhanced in-plane Mn-O hybridizations. The magnetic superexchange interaction is very sensitive to the polar bond-bending distortion, and we find that this dependence directly causes a strong magnetoelectric coupling. This novel mechanism for multiferroicity is consistent with the experimentally observed reduced ferroelectric polarization upon the onset o…
We consider phase separated states in magnetic oxides (MO) thin films. We show that these states have a non-zero electric polarization. Moreover, the polarization is intimately related to a spatial distribution of magnetization in the film. Polarized states with opposite polarization and opposite magnetic configuration are degenerate. An external electric field removes the degeneracy and allows to switch between the two states. So, one can control electric polarization and magnetic configuration of the phase separated MO thin film with the external electric field.
We study magnetic state and electron transport properties of composite multiferroic system consisting of a granular ferromagnetic thin film placed above the ferroelectric substrate. Ferroelectricity and magnetism in this case are coupled by the long-range Coulomb interaction. We show that magnetic state and magneto-transport strongly depend on temperature, external electric field, and electric polarization of the substrate. Ferromagnetic order exists at finite temperature range around ferroelectric Curie point. Outside the region the film is in the superparamagnetic state. We demonstrate that …
Our magnetic, electrical, and thermal measurements on single-crystals of the novel Mott insulator, Sr2IrO4, reveal a novel giant magneto-electric effect (GME) arising from a frustrated magnetic/ferroelectric state whose signatures are: (1) a strongly enhanced electric permittivity that peaks near a newly observed magnetic anomaly at 100 K, (2) a large (~100%) magneto-dielectric shift that occurs near a metamagnetic transition, and (3) magnetic and electric polarization hysteresis. The GME and electric polarization hinge on a spin-orbit gapping of 5d-bands, rather than the magnitude and spatial…
An ancient Hamiltonian of electrons with entangled spin and orbital degrees of freedom is re-examined as a model of magneto-electric multipoles. In the model, a magnetic charge and simple quantum rotator are tightly locked in action, some might say they are enslaved entities. It is shown that magneto-electric multipoles almost perfectly accord with those inferred from an analysis of magnetic neutron diffraction data on a ceramic superconductor (YBCO) in the pseudo-gap phase. Nigh on perfection between Stone's model and inferred magneto-electric multipoles is achieved by addition to the origina…
A new microscopic mechanism of the magneto-electric (ME) effect based on the spin supercurrent is theoretically presented for non-collinear magnets. The close analogy between the superconductors (charge current) and magnets (spin current) is drawn to derive the distribution of the spin supercurrent and the resultant electric polarization. Application to the spiral spin structure is discussed.
We present a theoretical examination of the magneto-electric response in the recently discovered multiferroic insulator Cu$_2$OSeO$_3$. Combining Monte Carlo simulation and Ginzburg-Landau analysis we predict the response in each of the magnetic phases, including helical, conical, ferromagnetic and Skyrmion crystal phases, both for thin film and bulk systems. A common feature for all non-collinear phases is that the magneto-electric susceptibility increases linearly with the applied magnetic field. Being both calculable and measurable, the magneto-electric susceptibility can serve as a new pow…
We succeed in deriving an exact expression for the magnetic interaction of neutrons and electrons including magneto-electric operators, allowed in the absence of a centre of inversion symmetry. Central characters are a spin anapole and an orbital (toroidal) analogue, in addition to familiar parity-even operators. A simulation of neutron diffraction by antiferromagnetic copper oxide makes full use of information inferred from a thorough investigation with resonant x-ray Bragg diffraction.
A theory that fully describes previously observed neutron Bragg spots indicative of magnetic order in the pseudo-gap phase of YBa2Cu3O6 + x is presented. Magnetic diffraction intensities, unveiled by polarization analysis, are explained by parity-violating magnetic (magneto-electric) quadrupoles at in-plane Cu sites arranged in a simple ferro-type motif. An absence of conventional spin and orbital angular momentum dipoles in the theory is compatible with the occurrence of superconductivity and strongly suggests, moreover, that magneto-electric quadrupoles are the primary order-parameter in the…
The magneto-electric (ME) coupling on spin-wave resonances in single-crystal Cu2OSeO3 was studied by a novel technique using electron spin resonance combined with electric field modulation. An external electric field E induces a magnetic field component μ_0 H^i = γE along the applied magnetic field H with γ=0.7(1) μT/(V/mm) at 10 K. We found that ME coupling strength γis temperature dependent and highly anisotropic. γ(T) nearly follows that of spin susceptibility J(T) and rapidly decreases above the Curie temperature Tc. The ratio γ/J monotonically decreases with increasing temperature without…
We propose a microscopic magneto-electric model in which the coupling between spins and electric dipoles is mediated by lattice distortions. The magnetic sector is described by a spin S=1/2 Heisenberg model coupled directly to the lattice via a standard spin-Peierls term and indirectly to the electric dipole variables via the distortion of the surrounding electronic clouds. Electric dipoles are described by Ising variables for simplicity. We show that the effective magneto-electric coupling which arises due to the interconnecting lattice deformations is quite efficient in one-dimensional array…
Collective mode dynamics of the helical magnets coupled to electric polarization via spin-orbit interaction is studied theoretically. The soft modes associated with the ferroelectricity are not the transverse optical phonons, as expected from the Lyddane-Sachs-Teller relation, but are the spin waves hybridized with the electric polarization. This leads to the Drude-like dielectric function $ε(ω)$ in the limit of zero magnetic anisotropy. There are two more low-lying modes; phason of the spiral and rotation of helical plane along the polarization axis. The roles of these soft modes in the neutr…
We present an element selective resonant magnetic x-ray scattering study of NdFe3(BO3)4 as a function of temperature and applied magnetic field. Our measurements show that the magnetic order of the Nd sublattice is induced by the Fe spin order. When a magnetic field is applied parallel to the hexagonal basal plane, the helicoidal spin order is suppressed and a collinear ordering, where the moments are forced to align in a direction perpendicular to the applied magnetic field, is stabilized. This result excludes a non-collinear spin order as the origin of the magnetically induced electric polar…
The ferroelectric order and magnetic field induced effects observed in the spiral phase of MnWO4 are described theoretically. It is demonstrated explicitly that the Dzyaloshinskii-Moriya antisymmetric interactions contribute to the correlation between spins and electric dipoles in the incommensurate and commensurate ferroelectric phases of magnetic multiferroics. However, other single-site symmetric interactions are shown to be involved in the magnetoelectric process, suggesting the possible existence of an electric polarization originating from purely symmetric effects.
Some magnetoelectric multiferroics have a canted spin structure that can be described by a Dzyaloshinkii-Moriya coupling. We calculate properties and features expected for surface and bulk magnon polaritons in such media with a linear magnetoelectric interaction for the case of transverse electric polarisation. The dielectric polarisation and magnetisation of weak ferromagnetism are constrained to lie in the plane parallel to the surface. We examine a geometry with the polarisation oriented in the film plane and present numerical results for the transverse electric polarisation. Particular att…
The chiral magneto-electric compound Ni3TeO6 is investigated through temperature-dependent synchrotron-based powder x-ray diffraction and x-ray absorption spectroscopy between 15 to 300 K. Our work provides direct evidence for the exchange-striction in the material around the concomitant onset point of collinear antiferromagnetic and magneto-electric phases. The x-ray absorption near edge spectra and x-ray photoelectron spectra show that the sample consists of both Ni2+ and Ni3+ ions in the lattice. The ionic state of Ni is found to be quite robust, and it is largely independent of the prepara…
The $J_1$-$J_2$ quantum spin sawtooth chain is a paradigmatic one-dimensional frustrated quantum spin system exhibiting unconventional ground-state and finite-temperature properties. In particular, it exhibits a flat energy band of one-magnon excitations accompanied by an enhanced magnetocaloric effect for two singular ratios of the basal interactions $J_1$ and the zigzag interactions $J_2$. In our paper, we demonstrate that one can drive the spin system into a flat-band scenario by applying an appropriate electric field, thus overcoming the restriction of fine-tuned exchange couplings $J_1$ a…
Magnetic, dielectric, and magnetoelectric properties in a spin-state transition system are examined, motivated by the recent discovery of a multiferroic behavior in a cobalt oxide. We construct an effective model Hamiltonian based on the two-orbital Hubbard model, in which the spin-state degrees of freedom in magnetic ions couple with ferroelectric-type lattice distortions. A phase transition occurs from the high-temperature low-spin phase to the low-temperature high-spin ferroelectric phase with accompanying an increase of the spin entropy. The calculated results are consistent with the exper…
We submit that the magnetic space-group Cac (#9.41) is consistent with the established magnetic structure of BaFe2Se3, with magnetic dipole moments in a motif that uses two ladders [Caron J M et al 2011 Phys. Rev. B 84 180409(R)]. The corresponding crystal class m1' allows axial and polar dipoles and forbids bulk ferromagnetism. The compound supports magneto-electric multipoles, including a magnetic charge (monopole) and an anapole (magnetic toroidal dipole) visible in the Bragg diffraction of x-rays and neutrons. Our comprehensive simulation of neutron Bragg diffraction by BaFe2Se3 exploits e…
Uniquely in Cu2OSeO3, the Skyrmions, which are topologically protected magnetic spin vortex-like objects, display a magnetoelectric coupling and can be manipulated by externally applied electric (E) fields. Here, we explore the E-field coupling to the magnetoelectric Skyrmion lattice phase, and study the response using neutron scattering. Giant E-field induced rotations of the Skyrmion lattice are achieved that span a range of $\sim$25$^{\circ}$. Supporting calculations show that an E-field-induced Skyrmion distortion lies behind the lattice rotation. Overall, we present a new approach to Skyr…
We report for the first time, that Fe3Se4 is a room temperature, type-II multiferroic with magnetoelectric coupling. We observed the coexistence of coupled ferrimagnetic and ferroelectric ordering in Fe3Se4nanorods well above room temperature, which is a hard magnet with large magnetocrystalline anisotropy. For the first time, we observed spontaneous, reversible ferroelectric polarization in Fe3Se4 nanorods below the magnetic Curie temperature. The coupling is manifested by an anomaly in the dielectric constant and Raman shift at Tc. We do not completely understand the origin of the ferroelect…
The transition metal thiophosphates $M$PS$_3$ ($M$ = Mn, Fe, Ni) are a class of van der Waals stacked insulating antiferromagnets that can be exfoliated down to the ultrathin limit. MnPS$_3$ is particularly interesting because its N$\acute{\textrm{e}}$el ordered state breaks both spatial-inversion and time-reversal symmetries, allowing for a linear magneto-electric phase that is rare among van der Waals materials. However, it is unknown whether this unique magnetic structure of bulk MnPS$_3$ remains stable in the ultrathin limit. Using optical second harmonic generation rotational anisotropy, …
Stimulated by recent studies of quantum phases with broken local inversion symmetry, we study the magnetoelectric effect in locally noncentrosymmetric metals. We consider three-dimensional (3D) coupled zigzag chains and demonstrate that the antiferromagnetic moment is induced by the electric current through a staggered antisymmetric spin-orbit coupling. This current-induced magnetism is much larger than that in globally noncentrosymmetric metals. We provide an intuitive understanding of the current-induced antiferromagnetic moment by showing the inverse magnetoelectric effect, that is, the fer…
We report on magnetisation and magneto-capacitance measurements in the Bi1-xLaxFeO3 series for 0 < x < 0.15. We confirm that doping with La reduces the threshold magnetic field Hc for cancelling the magnetic spiral phase, and we show that Hc decreases as the La content increases up to x=0.15, which is the highest concentration for maintaining the non-centrosymmetric rhombohedral structure of BiFeO3. Measurements of the dielectric constant as a function of magnetic field in the series also show a maximum magneto-capacitance for x=0.15.
Motivated by recent studies of odd-parity multipole order in condensed matter physics, we theoretically study magnetoelectric responses in an electric octupole state. Investigating the Edelstein effect and spin Hall effect in a locally noncentrosymmetric bilayer Rashba model, we clarify characteristic properties due to parity violation in the electric octupole state. Furthermore, a possible realization of electric octupole order in bilayer high-Tc cuprate superconductors is proposed. Our calculation of magnetic torque is consistent with recent experimental observation of a kink above the super…
It is argued that in magnetoelectrics with diagonal magnetoelectric coupling there should be a monopole-like distribution of magnetization around electric charge. It may lead to nontrivial transport properties of such materials, to understand which the picture of magnetic monopoles attached to electric charges may be very useful.
Magnetoelectric properties of a coupled spin-electron model on a doubly decorated square lattice in an external electric field applied along the crystallographic axis [11] are rigorously examined with the help of generalized decoration-iteration transformation. The phase diagram, spontaneous magnetization and electric polarization are exactly calculated and their dependencies are comprehensively investigated under a concurrent influence of temperature and electric field. It is found that the electric field mostly stabilizes at zero temperature the spontaneous antiferromagnetic order with respe…
We present a simple two-dimensional model in which the lattice degrees of freedom mediate the interactions between magnetic moments and electric dipoles. This model reproduces basic features, such as a sudden electric polarization switch-off when a magnetic field is applied and the ubiquitous dimerized distortion patterns and magnetic $\uparrow \uparrow \downarrow \downarrow$ ordering, observed in several multiferroic materials of different composition. The list includes E-type manganites, RMnO$_3$, nickelates such as in YNiO$_3$ and other materials under strain, such as TbMnO$_3$. In spite of…
