Electromagnons in multiferroic YMn2O5 and TbMn2O5

Based on temperature dependent far infrared transmission spectra of YMn2O5 and TbMn2O5 single crystals, we report the observation of electric dipole-active magnetic excitations, or electromagnons, in these multiferroics. Electromagnons are found to be directly responsible for the steplike anomaly of the static dielectric constant at the commensurate--incommensurate magnetic transition and are the origin of the colossal magneto-dielectric effect reported in these multiferroics.     

Magnetic excitations in the low-temperature ferroelectric phase of multiferroic YMn2O5 using inelastic neutron scattering

We studied magnetic excitations in a low-temperature ferroelectric phase of the multiferroic YMn(2)O(5) using inelastic neutron scattering (INS). We identify low-energy magnon modes and establish a correspondence between the magnon peaks observed by INS and electromagnon peaks observed in optical absorption [A. B. Sushkov et al., Phys. Rev. Lett. 98, 027202 (2007).]. Furthermore, we explain the microscopic mechanism, which results in the lowest-energy electromagnon peak, by comparing the inelastic neutron spectral weight with the polarization in the commensurate ferroelectric phase.     

Resonant soft X-ray scattering studies of multiferroic YMn2O5

We performed soft X-ray resonant scattering at the MnL _2,3- and OK edges of YMn₂O₅. While the resonant intensity at the Mn L _2,3 edges reflects the magnetic order parameter, the resonant scattering at the O K edge is found to be directly related to the macroscopic ferroelectric polarization. The latter observation reveals the important role of the spin-dependent Mn-O hybridization for the multiferroicity of YMn₂O₅. We present details about how to obtain correct energy dependent lineshapes and discuss the origin of the resonant intensity at the O K edge.     

Electronic correlations decimate the ferroelectric polarization of multiferroic homn2o5

We show that electronic correlations decimate the intrinsic ferroelectric polarization of multiferroic manganites RMn2O5, where R is a rare earth element. Such is manifest from ab initio band structure computations that account for the Coulomb interactions between the manganese 3d electrons--the root of magnetism in RMn2O5. Including these leads to an amplitude and direction of polarization of HoMn2O5 that agree with experiment. The decimation is caused by a near cancellation of the ionic polarization induced by the lattice and the electronic one due to valence charge redistributions.     

Electric field switching of antiferromagnetic domains in YMn2O5: a probe of the multiferroic mechanism

We employ neutron spherical polarimetry to determine the nature and population of the coexisting antiferromagnetic domains in multiferroic YMn2O5. By applying an electric field, we prove that reversing the electrical polarization results in the population inversion of two types of in-plane domains, related to each other by inversion. Our results are completely consistent with the exchange-striction mechanism of ferroelectricity, and support a unified model where cycloidal ordering is induced by coupling to the main magnetic order parameter.     

Ferroelectricity induced by acentric spin-density waves in YMn2O5

The commensurate and incommensurate magnetic structures of the magnetoelectric system YMn2O5, as determined from neutron diffraction, were found to be spin-density waves lacking a global center of symmetry. We propose a model, based on a simple magnetoelastic coupling to the lattice, which enables us to predict the polarization based entirely on the observed magnetic structure. Our data accurately reproduce the temperature dependence of the spontaneous polarization, particularly its sign reversal at the commensurate-incommensurate transition.     

Charge ordering of LuFe2O4 electronic multiferroic

Charge ordering of iron ions in LuFe2O4 frustrated electronic ferroelectric with variable valence is considered. Charge degrees of freedom are described in frameworks of Ising model with Coulomb interaction between sites. Mean field approximation is used to find free energies of the most probable structures. Phase diagrams of a single triangular bilayer and a system of triangular bilayers are plotted. A partially disordered dimer structure is proposed as a 2D high temperature phase. The transition from 2D to 3D ordering associated with a drop in temperature and the formation of spontaneous dipole moments is discussed.     

Magnetic reversal of the ferroelectric polarization in a multiferroic spinel oxide

Ferroelectric transition has been detected in a ferrimagnetic spinel oxide of CoCr2O4 upon the transition to the conical spin order below 25 K. The direction [110] of the spontaneous polarization is normal to both the magnetization easy axis [001] and to the propagation axis [110] of the transverse spiral component, in accord with the prediction based on the spin-current model. The reversal of the spontaneous magnetization by a small magnetic field (approximately 0.1 T) induces the reversal of the spontaneous polarization, indicating the clamping of the ferromagnetic and ferroelectric domain walls.     

Observation of multiferroic properties in pyroxene NaFeGe2O6

We report the observation of multiferroicity in a clinopyroxene NaFeGe(2)O(6) polycrystal from the investigation of its electrical and magnetic properties. Following the previously known first magnetic transition at T(N1) = 13 K, a second magnetic transition appears at T(N2) = 11.8 K in the temperature dependence of the magnetization. A ferroelectric polarization starts to develop clearly at T(N2) rather than T(N1) and its magnitude increases up to ~13 μC m(-2) at 5 K, supporting the idea that the ferroelectric state in NaFeGe(2)O(6) stems from a helical spin order stabilized below T(N2). When a magnetic field of 90 kOe is applied, the electric polarization decreases to 9 μC m(-2) and T(N2) slightly increases by 0.5 K. At intermediate magnetic fields, around 28 and 78 kOe, anomalies in the magnetoelectric current, magnetoelectric susceptibility, and field derivative of magnetization curves are found, indicating field-induced spin-state transitions. Based on these electrical and magnetic properties, we provide a detailed low temperature phase diagram up to 90 kOe, and discuss the nature of each phase of NaFeGe(2)O(6).     

Enhanced ferroelectric polarization by induced Dy spin order in multiferroic DyMnO3

Neutron powder diffraction and single crystal x-ray resonant magnetic scattering measurements suggest that Dy plays an active role in enhancing the ferroelectric polarization in multiferroic DyMnO3 above T(Dy)(N)=6.5 K. We observe the evolution of an incommensurate ordering of Dy moments with the same periodicity as the Mn spiral ordering. It closely tracks the evolution of the ferroelectric polarization. Below T(Dy)(N), where Dy spins order commensurately, the polarization decreases to values similar for those of TbMnO3. The higher P(s) found just above T(Dy)(N) arises from the contribution of Dy spins so as to effectively increase the amplitude of the Mn spin spiral.     

Charge-stripe order in the electronic ferroelectric LuFe2O4

The structural features of the charge ordering states in LuFe(2)O(4) are characterized by in situ cooling transmission electron microscopy observations from 300 K down to 20 K. Two distinctive structural modulations, a major q1=(1/3,1/3,2) and a weak q2 = q1/10+(0,0,3/2), have been well determined at the temperature of approximately 20 K. Systematic analysis demonstrates that the charges at low temperatures are well crystallized in a charge-stripe phase, in which the charge-density wave behavior in a nonsinusoidal fashion results in elemental electric dipoles for ferroelectricity. It is also noted that the charge ordering and ferroelectric domains often change markedly with lowering temperatures and yield a rich variety of structural phenomena.     

Electronic structure of YMn2O5 studied by EELS and first-principles calculations

The electronic structure of multiferroic YMn₂O₅ material has been studied by use of the generalized gradient approximation (GGA). The results demonstrate that the oxygen 2p and manganese 3d orbitals are strongly hybridized. Considering the on-site Coulomb interaction U, we performed the GGA+U calculations for 0 < U ? 8 eV, and it is found that the increase of U could enlarge the band gap and, on the other hand, weaken the Mn-O hybridization. The experimental measurements of the electron energy-loss spectrometry (EELS) exhibit a rich variety of structural features in both O-K edge and Mn-L edges. A theoretical and experimental analysis on the O-K edge suggests that the on-site Coulomb interaction (U) in YMn₂ O₅ could be less than 4 eV. Certain electronic structural features of LaMn₂O₅ have been discussed in comparison with those of YMn₂O₅.     

Molecular-spin dynamics study of electromagnons in multiferroic RMn2O5

We investigate the electromagnon in magnetoferroelectrics RMn(2)O(5) using combined molecular-spin dynamics simulations. We confirm that the origin of the electromagnon modes observed in the optical spectra is due to the exchange-striction interaction between the magnons and the phonons, and the dielectric step at the magnetic phase transition is due to the appearance of the electromagnon in the low-temperature phase in these materials. The magnetic anisotropy breaks the rotational symmetry of the magnetic structures and, as a result, the electromagnon splits into three modes in RMn(2)O(5). We find that the electromagnon frequencies are very sensitive to the magnetic wavevector along the a direction q(x). Therefore, the electromagnon frequencies of TmMn(2)O(5) (q(x) ~ 0.467) are expected to be much higher than those of other materials of the family, such as R= Tb, Y, Ho, etc (q(x) ~ 0.48). We further calculate the electromagnons in the magnetic field, and find a new mode appearing in the magnetic field. Although the modes' frequencies change significantly under magnetic field, the total static dielectric constant contributed from the electromagnons does not change much in the magnetic field, suggesting that the colossal magnetodielectric effects in these materials may not be caused by the electromagnons.     

Order parameters and phase diagram of multiferroic RMn2O5

The generic magnetic phase diagram of multiferroic RMn2O5 (with R=Y, Ho, Tb, Er, Tm), which allows different sequences of ordered magnetic structures for different R's and different control parameters, is described using order parameters which explicitly incorporate the magnetic symmetry. A phenomenological magnetoelectric coupling is used to explain why some of these magnetic phases are also ferroelectric. Several new experiments, which can test this theory, are proposed.     

Structural anomalies and multiferroic behavior in magnetically frustrated TbMn2O5

We have studied the magnetostructural phase diagram of multiferroic TbMn2O5 as a function of temperature and magnetic field by neutron diffraction. Dielectric and magnetic anomalies are found to be associated with steps in the magnetic propagation vector, including a rare example of a commensurate-incommensurate transition on cooling below 24 K, and in the structural parameters. The geometrically frustrated magnetic structure is stabilized by "canted antiferroelectric" displacements of the Mn3+ ions, an example of the magnetic Jahn-Teller effect. The Tb moments order ferromagnetically at low temperatures in an applied field, while the Mn magnetic structure is largely unchanged.     

Influence of cycling electric polarization on multiferroic behaviors in heterostructural films composed of ferroelectric and ferromagnetic oxides

The CoFe₂O₄/Pb(Zr_0.52Ti_0.48)O₃ bilayer films were prepared by a sol–gel process, and the influence of cycling electric polarization on the multiferroic behaviors of the bilayer films was studied. The ferroelectric polarization hysteresis loops under various choices of magnetic bias were measured by an integrating current method. The results showed that after undergoing cycling electric polarization the ferroelectric polarization of the bilayer films enhanced and the suppression of ferroelectric polarization by external magnetic bias remarkably weakened. Based on the measurements of activation energy and leakage current, we confirmed that the oxygen vacancy migration in the bilayer films occurred during cycling electric polarization. Furthermore, we analyzed the mechanism of the influence of cycling electric polarization on the multiferroic behaviors of the bilayer films and attributed it to the oxygen vacancy migration, which could cause a part of ferroelectric domains to be unpinned from the oxygen vacancies and become more active under electric field and magnetic bias.     

Manipulating the magnetic structure with electric fields in multiferroic ErMn2O5

Based on measurements of soft x-ray magnetic diffraction under in situ applied electric field, we report on significant manipulation and exciting of commensurate magnetic order in multiferroic ErMn2O5. The induced magnetic scattering intensity arises at the commensurate magnetic Bragg position whereas the initial magnetic signal almost persists. We demonstrate the possibility to imprint a magnetic response function in ErMn2O5 by applying an electric field.     

Magnetoelectric coupling in RMn2O5 multiferroic: a Monte Carlo simulation

Magnetoelectric coupling in RMn₂O₅ (with R?=?non magnetic) multiferroics have been studied using the Monte Carlo simulation. The variation of magnetization and the polarization of RMn₂O₅ multiferroic have been determined. The system undergoes a magnetic transition at T_N and a further reduction of the temperature leads to a ferroelectric transition at T_C?<_? T_N depending on the coupling strength. Magnetic and ferroelectric hysteresis loops are obtained for several temperatures values. Variation of polarization with the external magnetic field of RMn₂O₅ has been given. Variation of polarization and magnetization with the electric field of RMn₂O₅ has been obtained.     

Sequence of phase transitions in the thermal dissociation and hydrogen reduction of YMn2O5 Compound

The sequence of phase transitions in the thermal dissociation and hydrogen reduction of YMn₂O₅ compound in the temperature range of 973–1123 K at pressures of 10³-10^-16 Pa is determined by the static method on a vacuum circulation system with subsequent X-ray diffraction analysis of the quenched solid phases. A fragment of the isothermal cross section of the Y-Mn-O system phase diagram is constructed in composition-oxygen pressure coordinates at 1173 K.