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.     

Symmetry of multiferroicity in a frustrated magnet TbMn2O5

Based on measurements of soft-x-ray magnetic scattering and symmetry considerations, we demonstrate that the magnetoelectric effect in TbMn2O5 arises from an internal field determined by S-->q--> x S-->-q--> with S-->q--> being the magnetization at modulation vector q-->, whereas the magnetoelastic effect in the exchange energy governs the response to external electric fields. Our results set fundamental symmetry constraints on the microscopic mechanism of multiferroicity in frustrated magnets.     

Non-resonant and resonant x-ray scattering studies on multiferroic TbMn2O5

Comprehensive x-ray scattering studies, including resonant scattering at Mn L, Tb L, and M edges, were performed on single crystals of TbMn2O5 for crystallographic data to elucidate the nature of its commensurate and incommensurate phases. The scattering results provide direct evidence of symmetry lowering to the ferroelectric phase driven by magnetically induced lattice modulations and show the presence of multiple magnetic orders. The competing orders under spin-frustrated geometry are believed to cause discommensuration and result in the commensurate-to-incommensurate phase transition around 24 K. It is proposed that the low temperature incommensurate phase consists of commensurate domains separated by antiphase domain walls which change both signs of spontaneous polarizations and x-ray scattering amplitudes for forbidden reflections.     

Spin dynamics and magnetic order in magnetically frustrated Tb2Sn2O7

We report a study of the geometrically frustrated magnetic material Tb2Sn2O7 by the positive muon-spin relaxation technique. No signature of a static magnetically ordered state is detected while neutron magnetic reflections are observed in agreement with a published report. This is explained by the dynamical nature of the ground state of Tb2Sn2O7: the Tb3+ magnetic moment characteristic fluctuation time is approximately 10(-10) s. The strong effect of the magnetic field on the muon-spin-lattice relaxation rate at low fields indicates a large field-induced increase of the magnetic density of states of the collective excitations at low energy.     

Ferroelectricity driven by the noncentrosymmetric magnetic ordering in multiferroic TbMn(2)O(5): a first-principles study

The ground state structural, electronic, and magnetic properties of multiferroic TbMn(2)O(5) are investigated via first-principles calculations. We show that the ferroelectricity in TbMn(2)O(5) is driven by the noncentrosymmetric magnetic ordering, without invoking the spin-orbit coupling and noncollinear spins. The intrinsic electric polarization in this compound is calculated to be 1187 nC cm(-2), an order of magnitude larger than previously thought.     

Spin fluctuations in a magnetically frustrated metal LiV(2)O(4).

Inelastic neutron scattering is used to characterize spin fluctuations in the d-electron heavy fermion spinel LiV(2)O(4). The spin-relaxation rate, gamma(Q), for Q = 0.6 A(-1) is 1.4(2) meV at low temperatures and increases linearly with temperature at a rate of 0.46(8)k(B). There is antiferromagnetic short-range order at low temperatures with a characteristic wave vector Q(c) = 0.64(2) A(-1) and a correlation length of 6(1) A. While warming shifts intensity towards lower Q, the staggered susceptibility peaks at a finite wave vector for T < 80 K. The data are compared with conventional heavy fermion systems, geometrically frustrated insulating magnets, and recent theories for LiV(2)O(4).     

Observation of electronic ferroelectric polarization in multiferroic YMn2O5

We report the observation of a magnetic polarization of the O 2p states in YMn(2)O(5) through the use of soft x-ray resonant scattering at the oxygen K edge. Remarkably, we find that the temperature dependence of the integrated intensity of this signal closely follows the macroscopic electric polarization, and hence is proportional to the ferroelectric order parameter. This is in contrast with the temperature dependence observed at the Mn L(3) edge, which reflects the Mn magnetic order parameter. First-principles calculations provide a microscopic understanding of these results and show that a spin-dependent hybridization of O 2p and Mn 3d states results in a purely electronic contribution to the ferroelectric polarization, which can exist in the absence of lattice distortions.     

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.     

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.     

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.     

Raman scattering in the magnetically frustrated double perovskite Sr2YRuO6

The spin correlations and excitations of the Sr₂YRuO₆ double perovskite are investigated by means of Raman scattering, complemented by synchrotron X‐ray diffraction measurements. Anomalous softening of a breathing mode of the oxygen octahedra is observed below ~200 K, much above the long‐range antiferromagnetic ordering temperature, T_N1 = 32 K, due to a spin‐phonon coupling mechanism in the presence of magnetic correlations. A diffusive Raman signal is also observed, possibly associated with spin excitations within magnetically correlated regions. Our results point to a characteristic energy and temperature scale of ~25 meV/200 K below which unusual behavior associated with magnetic correlations is observed in this material. Copyright © 2013 John Wiley & Sons, Ltd.     

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.     

First-principles calculations on ferroelectricity and lattice dynamics of Type-II multiferroic SmMn2O5

In this work, we report on the structural, electronic, and ferroelectric properties of SmMn₂O₅ by using first-principles density functional theory plus on-site Coulomb interaction (DFT + U) calculations. A thorough analysis was preformed to reveal the competing characteristics of different high-temperature (T) phases and the polarization mechanism in the low-T multiferroic phase. We show that the structural characteristics of the high-T phases have a strong influence on the low-T multiferroicity. In addition to the spin-induced lattice distortion that reduces substantially the purely electronic ferroelectricity, the dominant polarization mechanism in low-T SmMn₂O₅ still originates from the electronic polarization. By performing mode decomposition of the Hellmann–Feynman forces and the lattice distortion induced by the q = (0.5, 0, 0) magnetic order, we find that the Raman-active A_g mode characterized by the Mn⁴⁺O₆ octahedron distortion and synergistic displacement of Mn³⁺ and Sm ions is of primary importance, while the infrared (IR)-active B_2u mode plays a secondary role. These findings provide a theoretical foundation for future studies concerning the enhanced magnetoelectric effects of SmMn₂O₅ due to its pure exchange–striction mechanism.     

Three-dimensional magnetic correlations in multiferroic LuFe2O4

We present single crystal neutron diffraction measurements on multiferroic LuFe(2)O(4). Magnetic reflections are observed below transitions at 240 and 175 K indicating that the magnetic interactions in LuFe(2)O(4) are three-dimensional in character. The magnetic structure is refined as a ferrimagnetic spin configuration below the 240 K transition. Below 175 K a significant broadening of the magnetic peaks is observed along with the buildup of a diffuse component to the magnetic scattering.     

Magnetoelectric effect in multiferroic NdMn_2O_5

We have measured the dielectric constant for NdMn_2O_5 in an external magnetic field to map out the magnetoelectric phase diagram. The phase diagram corresponds well with the previously reported data of neutron diffraction and magnetic susceptibility. Our main finding is the observation of a dielectric anomaly in the low temperature phase with a strong magnetoelectric effect, which is attributed to the independent Nd~(3+) ordering. Moreover, the absence of the dielectric anomaly in the paramagnetic phase is discussed, keeping in view the exchange interaction and its dependence on the rareearth R~(3+) ionic radius.     

High-temperature structural phase transition in the LiCu2O2 multiferroic

The results of thermogravimetric, X-ray diffraction, and electrical studies of LiCu₂O₂ single crystals in the temperature range 300–1100 K are presented. A reversible first-order phase transition between the orthorhombic and tetragonal phases is found to occur in these single crystals at T = 993 K. A pronounced peak on a differential thermal analysis curve and jumps in the unit cell parameters and the electrical resistivity are detected at the phase-transition temperature. The data on the crystal structure of LiCu₂O₂ and the phase transition-induced change in the entropy determined in this work are used to conclude that the revealed phase transition is caused by the ordering-disordering of Li⁺ and Cu²⁺ cations in their structural positions.     

Anomalous critical behavior of NaV2O5

The temperature dependences and critical behavior of the dielectric constant were studied in NaV₂O₅ along the c axis in a frequency range of 1 MHz-1GHz and a temperature range of 4.2–300 K. An analysis of the data obtained, along with literature data on the heat capacity, magnetic losses, and the ultrasound velocity, indicates that the various physical quantities demonstrate similar temperature dependences in the vicinity of the transition, which corroborates the conclusion on the universality of the critical behavior in NaV₂O₅. Deviations from the predictions of the standard theory of second-order phase transitions were found, such as the asymmetry of the critical behavior above and below the transition and the presence of an anomalous base line.     

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.     

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).