Theory of electromagnon in the multiferroic Mn perovskites: Vital role of higher harmonic components of the spiral spin order

We study theoretically the electromagnon and its optical spectrum (OS) of the terahertz-frequency regime in the magnetic-spiral-induced multiferroic phases of the rare-earth (R) Mn perovskites, RMnO3, taking into account the elliptical deformation or the higher harmonics of the spiral spin configuration, which has been missed so far. A realistic spin Hamiltonian, which gives phase diagrams in agreement with experiments, resolves a long standing puzzle, i.e., the double-peak structure of the OS with a larger low-energy peak originating from magnon modes hybridized with the zone-edge state. We also predict the magnon branches associated with the electromagnon, which can be tested by neutron-scattering experiment.Comment: 5 pages, 4 figure

Effect of ferroelectric layers on the magnetocapacitance properties of superlattices-based oxide multiferroics

A series of superlattices composed of ferromagnetic La$_{0.7}$Ca$_{0.3}$MnO$_3$ (LCMO) and ferroelectric/paraelectric Ba$_{1-x}$Sr$_x$TiO$_3$ (0$\leq$x$\leq$1) were deposited on SrTiO$_3$ substrates using the pulsed laser deposition. Films of epitaxial nature comprised of spherical mounds having uniform size are obtained. Magnetotransport properties of the films reveal a ferromagnetic Curie temperature in the range of 145-158 K and negative magnetoresistance as high as 30%, depending on the type of ferroelectric layers employed for their growth (\QTR{it}{i.e.} '\QTR{it}{x'} value). Ferroelectricity at temperatures ranging from 55 K to 105 K is also observed, depending on the barium content. More importantly, the multiferroic nature of the film is determined by the appearance of negative magnetocapacitance, which was found to be maximum around the ferroelectric transition temperature (3% per \QTR{it}{tesla}). These results are understood based on the role of the ferroelectric/paraelectric layers and strains in inducing the multiferroism.Comment: Accepted to Applied Physics Letter

Microscopic Model and Phase Diagrams of the Multiferroic Perovskite Manganites

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 functions of the R-ion radius, which contain two different multiferroic states, i.e. the ab-plane spin cycloid with ferroelectric polarization P//a and the bc-plane spin cycloid with P//c. The orthorhombic lattice distortion or the second-neighbor spin exchanges enhanced by this distortion exquisitely controls the keen competition between these two phases through tuning the SIA and DMI energies. This leads to a lattice-distortion-induced reorientation of P from a to c in agreement with the experiments. We also discuss spin structures in the A-type antiferromagnetic state, those in the cycloidal spin states, origin and nature of the sinusoidal collinear spin state, and many other issues.Comment: 23 pages, 19 figures. Recalculated results after correcting errors in the assignment of Dzyaloshinsky-Moriya vector

Pressure induced enhancement of ferroelectricity in multiferroic RRMn2_2O5_5(RR=Tb,Dy, and Ho)

Measurements of ferroelectric polarization and dielectric constant were done on $R$Mn$_2$O$_5$ ($R$=Tb, Dy, and Ho) with applied hydrostatic pressures of up to 18 kbar. At ambient pressure, distinctive anomalies were observed in the temperature profile of both physical properties at critical temperatures marking the onset of long range AFM order (T$_{N1}$), ferroelectricity (T$_{C1}$) as well as at temperatures when anomalous changes in the polarization, dielectric constant and spin wave commensurability have been previously reported. In particular, the step in the dielectric constant at low temperatures (T$_{C2}$), associated with both a drop in the ferroelectric polarization and an incommensurate magnetic structure, was shown to be suddenly quenched upon passing an $R$-dependent critical pressure. This was shown to correlate with the stabilization of the high ferroelectric polarization state which is coincident with the commensurate magnetic structure. The observation is suggested to be due to a pressure induced phase transition into a commensurate magnetic structure as exemplified by the pressure-temperature ($p$-$T$) phase diagrams constructed in this work. The $p$-$T$ phase diagrams are determined for all three compounds.Comment: 8 pages, 6 figures, submitted for review in Phys. Rev.

Electrically driven spin excitation in a ferroelectric magnet DyMnO_3

Temperature (5--250 K) and magnetic field (0--70 kOe) variations of the low-energy (1--10 meV) electrodynamics of spin excitations have been investigated for a complete set of light-polarization configurations for a ferroelectric magnet DyMnO$_3$ by using terahertz time-domain spectroscopy. We identify the pronounced absorption continuum (1--8 meV) with a peak feature around 2 meV, which is electric-dipole active only for the light $E$-vector along the a-axis. This absorption band grows in intensity with lowering temperature from the spin-collinear paraelectric phase above the ferroelectric transition, but is independent of the orientation of spiral spin plane ($bc$ or $ab$), as shown on the original $P_{\rm s}$ (ferroelectric polarization) $\parallel c$ phase as well as the magnetic field induced $P_{\rm s}\parallel a$ phase. The possible origin of this electric-dipole active band is argued in terms of the large fluctuations of spins and spin-current.Comment: New version, 11 pages including colored 8 figure

Observation of nuclei with energies 8-30 MeV per nucleon in the Earth's magnetosphere at the altitudes 350 KM

Observations of the flux of nuclei with an energy of IO MeV per nucleon on the Salyut-7 Station in September 1984 are presented. The observed flux is smaller by a factor of 50 than the flux detected in May, 1981

Polar phonons and spin excitations coupling in multiferroic BiFeO3 crystals

Raman scattering measurements on BiFeO3 single crystals show an important coupling between the magnetic order and lattice vibrations. The temperature evolution of phonons shows that the lowest energy E and A1 phonon modes are coupled to the spin order up to the Neel temperature. Furthermore, low temperature anomalies associated with the spin re-orientation are observed simultaneously in both the E phonon and the magnon. These results suggest that magnetostriction plays an important role in BiFeO3

The polarizability model for ferroelectricity in perovskite oxides

This article reviews the polarizability model and its applications to ferroelectric perovskite oxides. The motivation for the introduction of the model is discussed and nonlinear oxygen ion polarizability effects and their lattice dynamical implementation outlined. While a large part of this work is dedicated to results obtained within the self-consistent-phonon approximation (SPA), also nonlinear solutions of the model are handled which are of interest to the physics of relaxor ferroelectrics, domain wall motions, incommensurate phase transitions. The main emphasis is to compare the results of the model with experimental data and to predict novel phenomena.Comment: 55 pages, 35 figure

Reactivity of bulky tris(Phenylpyrazolyl) methanesulfonate copper(I) complexes towards small unsaturated molecules

Reaction of the tris(3-phenylpyrazolyl)methane sulfonate species (Tpms(Ph))Li with the copper(I) complex [Cu(MeCN)(4)][PF6] affords [Cu(Tpms(Ph))(MeCN)] 1. The latter, upon reaction with equimolar amounts of cyclohexyl-(CyNC) or 2,6-dimethylphenyl (XylNC) isocyanides, or excess CO, furnishes the corresponding Cu(I)complexes [Cu(Tpms(Ph))(CNR)] (R = Cy 2, Xyl 3) or [Cu(Tpms(Ph))(CO)] 4. The ligated isocyanide in 2 or 3 (or the acetonitrile ligand in 1)is displaced by 3-iminoisoindolin-1-one to afford 5, the first copper(I) complex containing an 3-iminoisoindolin-1-one ligand. The ligated acetonitrile in 1 undergoes nucleophilic attack by methylamine to give the amidine complex [Cu(Tpms(Ph)){MeC(NH)NHMe}] 6, whereas only the starting materials were recovered from the attempted corresponding reactions of 2 and 3 with methylamine. Complexes 1 or 6 form the trinuclear hydroxo-copper(II)species [(mu-Cu){Cu(mu-OH) (2)(Tpms(Ph))}(2)] 7 upon air oxidation in moist methanol. In all the complexes the scorpionate ligand facially caps the metal in the N,N,O-coordination mode

Effects of ac-field amplitude on the dielectric susceptibility of relaxors

The thermally activated flips of the local spontaneous polarization in relaxors were simulated to investigate the effects of the applied-ac-field amplitude on the dielectric susceptibility. It was observed that the susceptibility increases with increasing the amplitude at low temperatures. At high temperatures, the susceptibility experiences a plateau and then drops. The maximum in the temperature dependence of susceptibility shifts to lower temperatures when the amplitude increases. A similarity was found between the effects of the amplitude and frequency on the susceptibility.Comment: 8 pages, 7 figures, Phys. Rev. B (in July 1st