Magnetoelectric phase diagrams of the perovskite manganites, Eu1-xYxMnO3 and Gd1-xTbxMnO3, are theoretically studied. We first construct a microscopic model, and then analyze the model using the Monte-Carlo method. We reproduce the diagrams, which contain two different multiferroic states, i.e., the ab-plane spin cycloid with electric polarization P//a and the bc-plane spin cycloid with P//c. We reveal that their competition originates from a conflict between the single-ion anisotropy and the Dzyaloshinsky-Moriya interaction, which is controlled by the second-neighbor spin exchanges enhanced by the GdFeO3-type distortion. This leads to a P flop from a to c with increasing x in agreement with the experiments.
Many multiferroic materials, with various chemical compositions and crystal structures, have been discovered in the past years. Among these multiferroics, some perovskite manganites with ferroelectricity driven by magnetic orders are of particular interest. In these multiferroic perovskite manganites, not only their multiferroic properties are quite prominent, but also the involved physical mechanisms are very plenty and representative. In this Brief Review, we will introduce some recent theoretical and experimental progress on multiferroic manganites.
The phase diagram of quarter-hole-doped perovskite manganites is investigated using the doubleexchange model. An exotic striped type-II multiferroic phase, where 25% of the nearest-neighbor spin couplings are orthogonal to each other, is found in the narrow-bandwidth region. Comparing with the spiral-spin ordering phase of undoped manganites, the multiferroic Curie temperature of the new phase is estimated to be ~4 times higher, while the ferroelectric polarization is similar in magnitude. Our study provides a path for noncollinear spin multiferroics based on electronic self-organization, diff…
Charge-ordered rare earth manganites Nd0.5Ca0.5MnO3, La0.25Nd0.25Ca0.5MnO3, Pr0.7Ca0.3MnO3 and Pr0.6Ca0.4MnO3 are found to exhibit dielectric constant anomalies around the charge-ordering or the magnetic transition temperatures. Magnetic fields have a marked effect on the dielectric properties, indicating the presence of coupling between the magnetic and electrical order parameters. The observation of magnetoferroelectricity in these manganites is in accord with the recent theoretical predictions of Khomskii and coworkers.
Complete magnetoelectric (ME) phase diagrams of orthorhombic $R$MnO$_{3}$ with and without magnetic moments on the $R$ ions have been established. Three kinds of multiferroic ground states, the $ab$-cycloidal, the $bc$-cycloidal, and the collinear $E$-type phases, have been identified by the distinct ME responses. The electric polarization of the $E$-type phase dominated by the symmetric spin exchange ($bm{S}_{i} cdot bm{S}_{j}$) is more than 10 times as large as that of the $bc$-cycloidal phase dominated by the antisymmetric one ($bm{S}_{i} times bm{S}_{j}$), and the ME response is enhanced n…
Multiferroic rare earth manganites attracted recent attention because of the coexistence of different types of magnetic and ferroelectric orders resulting in complex phase diagrams and a wealth of physical phenomena. The coupling and mutual interference of the different orders and the large magnetoelectric effect observed in several compounds are of fundamental interest and bear the potential for future applications in which the dielectric (magnetic) properties can be modified by the onset of a magnetic (dielectric) transition or the application of a magnetic (electric) field. The physical mec…
In this contribution to the special issue on multiferroics we focus on multiferroicity driven by different forms of charge ordering. We will present the generic mechanisms by which charge ordering can induce ferroelectricity in magnetic systems. There is a number of specific classes of materials for which this is relevant. We will discuss in some detail $(i)$ perovskite manganites of the type (PrCa)MnO$_3$, $(ii)$ the complex and interesting situation in magnetite Fe$_3$O$_4$, $(iii)$ strongly ferroelectric frustrated LuFe$_2$O$_4$, $(iv)$ an example of a quasi one-dimensional organic system. …
The behavior of the low-frequency electromagnon in multiferroic DyMnO3 has been investigated in external magnetic fields and in a magnetically ordered state. Significant softening of the electromagnon frequency is observed for external magnetic fields parallel to the a-axis (BIIa), revealing a number of similarities to a classical soft mode behavior known for ferroelectric phase transitions. The softening of the electromagnon yields an increase of the static dielectric permittivity which follows a similar dependence as predicted by the Lyddane-Sachs-Teller relation. Within the geometry BIIb th…
We discuss the particle size driven tunability of the coexistence of ferromagnetism and ferroelectricity in Pr0.67Ca0.33MnO3(PCMO) with the help of x ray diffraction, magnetization, impedance spectroscopy, and remanent polarization measurements. The remanent polarization measurements using the positive up negative down method clearly prove the existence of ferroelectricity in PCMO with phase separation between Zener polaron(ZP) ordered P21nm and disordered Pbnm structures. We also find that the ferroelectric response is enhanced in nanocrystalline samples so long as ZP ordering is not destroye…
Orthorhombically distorted perovskite manganites, RMnO3 with R being a trivalent rare-earth ion, exhibit a variety of magnetic and electric phases including multiferroic (i.e. concurrently magnetic and ferroelectric) phases and fascinating magnetoelectric phenomena. We theoretically study the phase diagram of RMnO3 by constructing a microscopic spin model, which includes not only the superexchange interaction but also the single-ion anisotropy (SIA) and the Dzyaloshinsky-Moriya interaction (DMI). Analysis of this model using the Monte-Carlo method reproduces the experimental phase diagrams as …
Magnetodielectric materials are characterized by a strong coupling of magnetic and dielectric properties and in rare cases simultaneously exhibit both, magnetic and polar order. Among other multiferroics, TbMnO3 and GdMnO3 reveal a strong magneto-dielectric (ME) coupling and as a consequence fundamentally new spin excitations exist: Electro-active magnons, or electromagnons, i. e. spin waves which can be excited by ac electric fields. Here we show that these excitations appear in the phase with an incommensurate (IC) magnetic structure of the manganese spins. In external magnetic fields this I…
We present a detailed dielectric study of the relaxation effects that occur in several perovskite rare-earth manganites, including the multiferroics TbMnO3 and DyMnO3. We demonstrate that the strong magnetocapacitive effects, observed for electrical fields E||c, are nearly completely governed by magnetic-state induced changes of the relaxation parameters. The multiferroic materials, which undergo a transition into a spiral magnetic state, show qualitatively different relaxation behavior than those compounds transferring into an A-type antiferromagnetic state. We ascribe the relaxations in both…
All-electrical control of a dynamic magnetoelectric effect is demonstrated in a classical multiferroic manganite DyMnO3, a material containing coupled antiferromagnetic and ferroelectric orders. Due to intrinsic magnetoelectric coupling with electromagnons a linearly polarized terahertz light rotates upon passing through the sample. The amplitude and the direction of the polarization rotation are defined by the orientation of ferroelectric domains and can be switched by static voltage. These experiments allow the terahertz polarization to be tuned using the dynamic magnetoelectric effect.
Hexagonal manganites are multiferroic materials with two highly-dissimilar phase transitions: a ferroelectric transition (from P63/mmc to P63cm) at a temperature higher than 1000 K and an antiferromagnetic transition at TN=65 - 130 K. Despite its critical relevance to the intriguing ferroelectric domain physics, the details of the ferroelectric transition are yet not well known to date primarily because of the ultra-high transition temperature. Using high-temperature X-ray diffraction experiments, we show that the ferroelectric transition is a single transition of abrupt order and R-Op displac…
We performed magnetic and ferroelectric measurements, associated with Landau theory and symmetry analysis, in order to clarify the situation of the YMnO3 system, a classical example of type I multiferroics. We found that the only magnetic group compatible with all experimental data (neutrons scattering, magnetization,polarization, dielectric constant, second harmonic generation) is the P6'3 group. In this group a small ferromagnetic component along c is induced by the Dzyaloshinskii-Moriya interaction, and observed here in SQUID magnetization measurements. We found that the ferromagnetic and a…
We demonstrate that dynamics of the ab-spiral-spin order in a magnetoelectric multiferroic Eu0.55Y0.45MnO3 can be unambiguously probed through optical second harmonic signals, generated via the spin-induced ferroelectric polarization. In the case of relatively weak photoexcitation,the ferroelectric and the spiral-spin order remains interlocked, both relaxing through spin-lattice relaxation in the non-equilibrium state. When the additional optical pulse illuminating sample is intense enough to induced a local phase transition thermally, the system creates a metastable state of the bc-spiral-spi…
The magnetic-field-induced 90-degree flop of ferroelectric polarization P in a spin-spiral multiferroic material TbMnO3 is theoretically studied based on a microscopic spin model. We find that the direction of the P-flop or the choice of +Pa or -Pa after the flop is governed by magnetic torques produced by the applied magnetic field H acting on the Mn spins and thus is selected in a deterministic way, in contradistinction to the naively anticipated probabilistic flop. This mechanism resolves a puzzle of the previously reported memory effect in the P direction depending on the history of the ma…
The field-induced multiferroic transition in TbMnO3 has been studied by neutron scattering. Apart strong hysteresis, the magnetic transition associated with the flop of electronic polarization exhibits a memory effect: after a field sweep, TbMnO3 does not exhibit the same phase as that obtained by zero-field cooling. The strong changes in the magnetic excitations across the transition perfectly agree with a rotation of the cycloidal spiral plane indicating that the inverse Dzyaloshinski-Moriya coupling causes the giant magnetoelectric effect at the field-induced transition. The analysis of the…
We have investigated electrically-active magnetic excitations (electromagnons) in perovskite manganites with the $E$-type (up-up-down-down) spin structure by terahertz spectroscopy. Eu$_{1-x}$Y$_x$MnO$_3$ (0.1$\le x\le$1) and Y$_{1-y}$Lu$_y$MnO$_3$ (0$\le y\le$1) without magnetic $f$-moments, which host collinear sinusoidal, $A$-type, cycloidal, and $E$-type spin orders, are used to examine the systematics of possible electromagnons. Three-peak structures (23, 35, 45 cm$^{-1}$) of magnetic origin show up in the $E$-type phase with little composition ($y$) dependence of frequencies, making a co…
The origin of the spiral spin-order in perovskite multiferroic manganites $R$MnO$_{3}$ ($RE=$ Tb or Dy) is here investigated using a two $e_{\rm g}$-orbitals double-exchange model. Our main result is that the experimentally observed spiral phase can be stabilized by introducing a relatively weak next-nearest-neighbor superexchange coupling ($\sim10%$ of the nearest-neighbor superexchange). Moreover, the Jahn-Teller lattice distortion is also shown to be essential to obtain a realistic spiral period. Supporting our conclusions, the generic phase diagram of undoped perovskite manganites is obtai…
Using in-field single crystal neutron diffraction we have determined the magnetic structure of TbMnO3 in the high field P||a phase. We unambiguously establish that the ferroelectric polarization arises from a cycloidal Mn spins ordering, with spins rotating in the ab plane. Our results demonstrate directly that the flop of the ferroelectric polarization in TbMnO3 with applied magnetic field is caused from the flop of the Mn cycloidal plane.
Recent spectroscopic studies at terahertz frequencies for a variety of multiferroics endowed with both ferroelectric and magnetic orders have revealed the possible emergence of a new collective excitation, frequently referred to as electromagnon. It is magnetic origin, but becomes active in response to the electric field component of light. Here we give an overview on our recent advance in the terahertz time-domain spectroscopy of electromagnons or electric-dipole active magnetic resonances, focused on perovskite manganites--$R$MnO$_3$ ($R$ denotes rare-earth ions). The respective electric and…
Ferroelectric spiral magnets DyMnO3 and TbMnO3 show similar behavior of electric polarization in applied magnetic fields. Studies of the field dependence of lattice modulations on the contrary show a completely different picture. Whereas in TbMnO3 the polarization flop from P||c to P||a is accompanied by a sudden change from incommensurate to commensurate wave vector modulation, in DyMnO3 the wave vector varies continuously through the flop transition. This smooth behavior may be related to the giant magnetocapacitive effect observed in DyMnO3.
We present a comprehensive single crystal neutron diffraction investigation of the $\rm Mn_{1-x}Co_{x}WO_4$ with $0.02\leq x \leq0.30$. At lower concentration $x \leq 0.05$, the system is quickly driven into the multiferroic phase with spin structure forming an elliptical spiral order similar to the parent compound. The reduction of electric polarization is ascribed to the tilting of the spiral plane. For $x\sim 0.075$, the magnetic structure undergoes a spin flop transition that is characterized by a sudden rotation of the spin helix envelope into the $ac$ plane. This spin structure persists …
Obtaining strong magnetoelectric couplings in bulk materials and heterostructures is an ongoing challenge. We demonstrate that manganite heterostructures of the form ${\rm (Insulator)/(LaMnO_3)_n/(CaMnO_3)_n/(Insulator)}$ show strong multiferroicity in magnetic manganites where ferroelectric polarization is realized by charges leaking from ${\rm LaMnO_3}$ to ${\rm CaMnO_3}$ due to repulsion. Here, an effective nearest-neighbor electron-electron (electron-hole) repulsion (attraction) is generated by cooperative electron-phonon interaction. Double exchange, when a particle virtually hops to its …
We have investigated dielectric properties in a series of crystals of $R$MnO$_{3}$ ($R$ is a rare earth ion) under magnetic fields and quasihydrostatic pressure. We have found that ferroelectric phase appeared in GdMnO$_3$ crystal below 13K. We have confirmed that a small spontaneous polarization exists along a axis ($P_a$) in the orthorhombic $Pbnm$ setting and that $P_a$ can be reversed by the dc electric field. The dielectric anomaly due to the ferroelectric transition accompanied thermal hysteresis and lattice striction. The ferroelectric transition temperature decreased with quasihydrosta…
We show that electronic correlations decimate the intrinsic ferroelectric polarization of the recently discovered class of multiferroic manganites RMn$_2$O$_5$, where R is a rare earth element. Such is manifest from {\it ab initio} bandstructure computations that account for the strong local Coulomb interactions between the manganese 3d electrons --the root of magnetism in these materials. When including these the computed electronic, magnetic and lattice structure of multiferroic HoMn$_2$O$_5$ results in an amplitude and direction of polarization that is in accordance with experiment. The mic…
A series of manganites Tb1-xHoxMnO3 (0<=x<=0.6) with orthorhombic structure are synthesized and detailed investigations on their multiferroicity are performed. Successive magnetic transitions upon temperature variation are evidenced for all samples, and both the Mn3+ spiral spin ordering and rare-earth spin ordering are suppressed with increasing x. Significant enhancement of both the polarization and magnetoelectric response within 0.2<x<0.4 is observed, which may be ascribed to the competition possibly existing between spiral and E-type spin orders. Theoretical calculation is given based on …
The double exchange model describing the coupling between conduction electrons and localized magnetic moments is relevant for a large family of physical systems including manganites. Here we reveal that the one dimensional double exchange model with an incommensurate magnetic elliptical spiral is a topological insulator with a Chern number $2\mathbb{Z}$ in the two dimensional space with one physical dimension and one ancillary dimension spanned by the Goldstone mode of the spiral. Moreover, the electronic states can be localized for a strong local exchange coupling. The topological protected e…
We report on structural, magnetic, dielectric, and thermodynamic properties of (Eu:Y)MnO3 for Y doping levels 0 <= x < 1. This system resembles the multiferroic perovskite manganites RMnO3 (with R= Gd, Dy, Tb) but without the interference of magnetic contributions of the 4f-ions. In addition, it offers the possibility to continuously tune the influence of the A-site ionic radii. For small concentrations x <= 0.1 we find a canted antiferromagnetic and paraelectric groundstate. For higher concentrations x <= 0.3 ferroelectric polarization coexists with the features of a long wavelength incommens…
Magnetic and dielectric properties with varying magnitude and direction of magnetic field H have been investigated for a triangular lattice helimagnet MnI2. The in-plane electric polarization P emerges in the proper screw magnetic ground state below 3.5 K, showing the rearrangement of six possible multiferroic domains as controlled by the in-plane H. With every 60-degree rotation of H around the [001]-axis, discontinuous 120-degree flop of P-vector is observed as a result of the flop of magnetic modulation vector q. With increasing the in-plane H above 3 T, however, the stable q-direction chan…
By means of symmetry analysis, density functional theory calculations, and Monte Carlo simulations we show that goethite, $α$-FeOOH, is a linear magnetoelectric below its Néel temperature $T_{\rm N}=400$ K. The experimentally observed magnetic field induced spin-flop phase transition results in either change of direction of electric polarization or its suppression. Calculated value of magnetoelectric coefficient is 0.24 $μ$C m$^{-2}$ T$^{-1}$. The abundance of goethite in nature makes it arguably the most widespread magnetoelectric material.
We summarize the existing experimental data on electromagnons in multiferroic RMn2O5 compounds, where R denotes a rare earth ion, Y or Bi, and discuss a realistic microscopic model of these materials based on assumption that the microscopic mechanism of magnetically-induced ferroelectricity and electromagnon absorption relies entirely on the isotropic Heisenberg exchange and magnetostrictive coupling of spins to a polar lattice mode and does not involve relativistic effects. This model explains many magnetic and optical properties of RMn2O5 manganites, such as the spin re-orientation transitio…
Chirality, i.e., the right- and left-handedness of structure, is one of the key concepts in many fields of science including biology, chemistry and physics, and its manipulation is an issue of vital importance. The electron spins in solids can form chiral configurations. In perovskite manganites RMnO3 (R=Tb, Dy,...etc), the Mn-spins form a cycloidal structure, which induces ferroelectric polarization (P) through the relativistic spin-orbit interaction. This magnetism-induced ferroelectricity (multiferroics) and associated infrared-active spin waves (electromagnons) open a promising route to co…
Obtaining strong magnetoelectric couplings in bulk materials and heterostructures is an ongoing challenge. We demonstrate that manganite heterostructures of the form ${\rm (Insulator)/(LaMnO_3)_n/(CaMnO_3)_n/(Insulator)}$ show strong multiferroicity in magnetic manganites where ferroelectric polarization is realized by charges leaking from ${\rm LaMnO_3}$ to ${\rm CaMnO_3}$ due to repulsion. Here, an effective nearest-neighbor electron-electron (electron-hole) repulsion (attraction) is generated by cooperative electron-phonon interaction. Double exchange, when a particle virtually hops to its …
Ferroelectric properties in magnetic fields of varying magnitude and direction have been investigated for a triangular-lattice helimagnet CuFe1-xGaxO2 (x=0.035). The magnetoelectric phase diagrams were deduced for magnetic fields along [001], [110], and [1-10] direction, and the in-plane magnetic field was found to induce the rearrangement of six possible multiferroic domains. Upon every 60-degree rotation of in-plane magnetic field around the c-axis, unique 120-degree flop of electric polarization occurs as a result of the switch of helical magnetic q-vector. The chirality of spin helix is al…
The experimental observation of multiferroic behavior in perovskite manganites with a spiral spin structure demands to clarify the origin of these magnetic states and their relation to ferroelectricity. We show that spin-spiral phases with diagonal wavevector and also the E-type phase exist for intermediate values of the Hund's rule and the Jahn-Teller coupling in the orbitally ordered and insulating state of the standard two-band model Hamiltonian for manganites. Our results support the spin-current mechanism for ferroelectricity and present an alternative view to earlier conclusions where fr…
By calculating the electronic, orbital, magnetic and lattice structure of half-doped manganites we establish the central role of oxygen buckling caused by the tilting of the MnO$_6$ octahedra -- in essence a steric effect. The buckling itself does not change the Mn-Mn bonds. Instead it drives the system towards an instability where these bonds can dimerize. In presence of electron-electron interactions, this instability can fully develop and beyond a critical buckling a Zener polaron groundstate with dimerized spins, lattice and orbitals forms spontaneously, resulting in a multiferroic state.
We have used in-field neutron and X-ray single crystal diffraction to measure the incommensurability δ of the crystal and magnetic structure of multiferroic TbMnO3 . We show that the flop in the electric polarization at the critical field HC, for field H along the a− and b−axis coincides with a 1st order transition to a commensurate phase with propagation vector κ = (0, 1/4, 0). In-field X-ray diffraction measurements show that the quadratic magneto-elastic coupling breaks down with applied field as shown by the observation of the 1st harmonic lattice reflections above an…
We report on the high pressure synthesis of BiMn$_7$O$_{12}$, a manganite displaying a "quadruple perovskite" structure. Structural characterization of single crystal samples shows a distorted and asymmetrical coordination around the Bi atom, due to presence of the $6s^{2}$ lone pair, resulting in non-centrosymmetric space group Im, leading to a permanent electrical dipole moment and ferroelectric properties. On the other hand, magnetic characterization reveals antiferromagnetic transitions, in agreement with the isostructural compounds, thus evidencing two intrinsic properties that make BiMn$…
In contrast to well studied multiferroic manganites with a spiral structure, the electric polarization in multiferroic borates is induced within collinear antiferromagnetic structure and can easily be switched by small static fields. Because of specific symmetry conditions, static and dynamic properties in borates are directly connected, which leads to giant magnetoelectric and magnetodielectric effects. Here we prove experimentally that the giant magnetodielectric effect in samarium ferroborate SmFe3(BO3)4 is of intrinsic origin and is caused by an unusually large electromagnon situated in th…
We investigate the possibility of controlling the magnetic phase transition of the heterointerface between a half-doped manganite La$_{0.5}$Ca$_{0.5}$MnO$_{3}$ and a multiferroic BiFeO$_{3}$ through magnetoelectric coupling. Using macroscopic magnetometry and element-selective x-ray magnetic circular dichroism at the Mn and Fe \emph{L}-edges, we discover that the ferroelectric polarization of BFO controls simultaneously the magnetization of BFO and LCMO. X-ray absorption spectra at oxygen \emph{K}-edge and linear dichroism at Mn \emph{L}-edge suggest that the interfacial coupling is mainly der…
Colossal magnetoresistance (CMR) and electroresistance (CER) induced by the electric field in spinel multiferroic CdCr2S4 are reported. It is found that a metal-insulator transition (MIT) in CdCr2S4 is triggered by the electrical field. In magnetic fields, the resistivity of CdCr2S4 responds similarly to that of CMR manganites. Combing previous reports, these findings make CdCr2S4 the unique compound to possess all four properties of the colossal magnetocapacitive (CMC), colossal electrocapacitive (CEC), CER, and CMR. The present results open a new venue for searching new materials to show CMR…
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…
In this proceeding, recent theoretical investigations by the authors on the multiferroic $R$MnO$_3$ perovskites are briefly reviewed at first. Using the double-exchange model, the realistic spiral spin order in undoped manganites such as TbMnO$_3$ and DyMnO$_3$ is well reproduced by incorporating a weak next-nearest neighbor superexchange ($\sim10%$ of nearest neighbor superexchange) and moderate Jahn-Teller distortion. The phase transitions from the A-type antiferromagnet (as in LaMnO$_3$), to the spiral phase (as in TbMnO$_3$), and finally to the E-type antiferromagnet (as in HoMnO$_3$), wit…
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 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…
The double exchange (DE) model is systematically applied for studying the coupling between ferroelectric (FE) and magnetic orders in several prototypical types of multiferroic manganites. The model was constructed for the magnetically active Mn $3d$ bands in the basis of Wannier functions and include the effect of screened on-site Coulomb interactions. The essence of our approach for the FE polarization is to use the Berry phase theory, formulated in terms of occupied Wannier functions, and to evaluate the asymmetric spin-dependent change of these functions in the framework of the DE model. Th…
We discuss theoretically frustrated Heisenberg spiral magnets in magnetic field $\bf H$. We demonstrate that small anisotropic spin interactions (single-ion biaxial anisotropy or dipolar forces) select the plane in which spins rotate (spiral plane) and can lead to the spiral plane flop upon in-plane field increasing. Expressions for the critical fields $H_{flop}$ are derived. It is shown that measuring of $H_{flop}$ is an efficient and simple method of quantifying the anisotropy in the system (as the measurement of spin-flop fields in collinear magnets with axial anisotropy). Corresponding rec…
Hexagonal Dy(0.5)Y(0.5)MnO3, a multiferroic rare-earth manganite with geometrically frustrated antiferromagnetism, has been investigated with single-crystal neutron diffraction measurements. Below 3.4 K magnetic order is observed on both the Mn (antiferromagnetic) and Dy (ferrimagnetic) sublattices that is identical to that of undiluted hexagonal DyMnO3 at low temperature. The Mn moments undergo a spin reorientation transition between 3.4 K and 10 K, with antiferromagnetic order of the Mn sublattice persisting up to 70 K; the antiferromagnetic order in this phase is distinct from that observed…
Magnetic excitations in cycloidal magnet LiCu$_2$O$_2$ are explored using THz absorption spectroscopy in magnetic fields up to 12 T. Below the spin ordering temperature we observe eight optically active transitions in the spin system of LiCu$_2$O$_2$ in the energy range from 4 to 30 cm$^{-1}$. In magnetic field the number of modes increases and the electric polarization flop is seen as a change in magnetic field dependence of mode energies. The polarization dependence of two of the modes in zero magnetic field fits the selection rules for the cycloid tilted by $θ=41\pm1^{\circ}$ from the bc pl…
We present the electron spin resonance study of the influence of an electric field on the low-field multiferroic magnetic state in LiCuVO4. The shift of the magnetic resonance spectra in the electric field has been observed experimentally. Symmetry analysis has been conducted in order to describe the static properties of the magnetic system. The low-frequency dynamics of LiCuVO4 in magnetic and electric fields was considered in the framework of hydrodynamic approach. It was shown that the application of the external electric field leads to the change of the configuration of the magnetic system…
The complete magnetic and multiferroic phase diagram of Mn$_{1-x}$Co$_{x}$WO$_4$ single crystals is investigated by means of magnetic, heat capacity, and polarization experiments. We show that the ferroelectric polarization $\overrightarrow{P}$ in the multiferroic state abruptly changes its direction twice upon increasing Co content, x. At x$_{c1}$=0.075, $\overrightarrow{P}$ rotates from the $b-$axis into the $a-c$ plane and at x$_{c2}$=0.15 it flips back to the $b-$axis. The origin of the multiple polarization flops is identified as an effect of the Co anisotropy on the orientation and shape…
Through a combination of neutron diffraction and Landau theory we describe the spin ordering in the ground state of the quadruple perovskite manganite CaMn7O12 - a magnetic multiferroic supporting an incommensurate orbital density wave that onsets above the magnetic ordering temperature, TN1 = 90 K. The multi-k magnetic structure in the ground state was found to be a nearly-constant-moment helix with modulated spin helicity, which oscillates in phase with the orbital occupancies on the Mn3+ sites via trilinear magneto-orbital coupling. Our phenomenological model also shows that, above TN2 = 48…
We investigate the possible types of coupling between ferroelectricity and magnetism for the zig-zag spin chain multiferroic LiCu2O2 compound. We construct a multi-order parameter phenomenological model for the material based on a group theoretical analysis. From our calculation we conclude that a coupling involving the inter-chain magnetic structure and ferroelectricity is necessary to understand the experimental results of Park et.al. Our proposed model is able to account for the electric polarization flop in the presence of an externally applied magnetic field. Furthermore, based on our the…
We demonstrate a new approach for directly measuring the ultrafast energy transfer between elec- trons and magnons, enabling us to track spin dynamics in an antiferromagnet (AFM). In multiferroic HoMnO3, optical photoexcitation creates hot electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced transparency, which builds up over several picoseconds as the spins heat up due to energy transfer from hot elec- trons via phonons. This spin-lattice thermalization time is ?10 times faster than that of typical ferromagnetic …
The optical spectra in the family of multiferroic manganites RMnO3 is a great puzzle. Current models can not explain the fact that two strong electromagnons are present in the non-collinear spin cycloidal phase, with only one electromagnon surviving the transition into the collinear spin sinusoidal phase. We show that this is a signature of the presence of anomalous magnetoelectric coupling that breaks rotational invariance in spin space and generates oscillatory polarization in the ground state.
