Optical control of magnetization of micron-size domains in antiferromagnetic NiO single crystals

We propose Raman-induced collinear difference-frequency generation (DFG) as a method to manipulate dynamical magnetization. When a fundamental beam propagates along a threefold rotational axis, this coherent second-order optical process is permitted by angular momentum conservation through the rotational analogue of the Umklapp process. As a demonstration, we experimentally obtained polarization properties of collinear magnetic DFG along a [111] axis of a single crystal of antiferromagnetic NiO with micro multidomain structure, which excellently agreed with the theoretical prediction.Comment: 11 pages, 3 figures, submitted to Physical Review Letter

A Field-Induced Re-Entrant Novel Phase and A Ferroelectric-Magnetic Order Coupling in HoMnO3

A re-entrant novel phase has been observed in the hexagonal ferroelectric HoMnO3 in the presence of magnetic fields, in the temperature ranges defined by the plateau of the dielectric constant anomaly. The dielectric plateau evolves with fields from a narrow sharp dielectric peak at the Mn-spin rotation transition at 32.8 K in zero magnetic field. Such a field-induced dielectric plateau anomaly appears both in the temperature sweep at a constant field and in the field sweep at a constant temperature without detectable hysteresis. This is attributed to the indirect coupling between the ferroelectric and antiferromagnetic orders, arising from an antiferromagnetic domain wall effect, where the magnetic order parameter of the Mn subsystem has to change sign across the ferroelectric domain wall in the compound, that influences the ferroelectric domains via a local magnetostrictive effect

Giant Magnetoelectric Effect in a Multiferroic Material with a High Ferroelectric Transition Temperature

We present a unique example of giant magnetoelectric effect in a conventional multiferroic HoMnO3, where polarization is very large (~56 mC/m2) and the ferroelectric transition temperature is higher than the magnetic ordering temperature by an order. We attribute the uniqueness of the giant magnetoelectric effect to the ferroelectricity induced entirely by the off-center displacement of rare earth ions with large magnetic moments. This finding suggests a new avenue to design multiferroics with large polarization and higher ferroelectric transition temperature as well as large magnetoelectric effects

Magnetically driven ferroelectric order in Ni3_3V2_2O8_8

We show that for Ni$_3$V$_2$O$_8$ long-range ferroelectric and incommensurate magnetic order appear simultaneously in a single phase transition. The temperature and magnetic field dependence of the spontaneous polarization show a strong coupling between magnetic and ferroelectric orders. We determine the magnetic symmetry of this system by constraining the data to be consistent with Landau theory for continuous phase transitions. This phenomenological theory explains our observation the spontaneous polarization is restricted to lie along the crystal b axis and predicts that the magnitude should be proportional to a magnetic order parameter.Comment: 11 pages, 3 figure

Second harmonic generation on incommensurate structures: The case of multiferroic MnWO4

A comprehensive analysis of optical second harmonic generation (SHG) on an incommensurate (IC) magnetically ordered state is presented using multiferroic MnWO4 as model compound. Two fundamentally different SHG contributions coupling to the primary IC magnetic order or to secondary commensurate projections of the IC state, respectively, are distinguished. Whereas the latter can be described within the formalism of the 122 commensurate magnetic point groups the former involves a breakdown of the conventional macroscopic symmetry analysis because of its sensitivity to the lower symmetry of the local environment in a crystal lattice. Our analysis thus foreshadows the fusion of the hitherto disjunct fields of nonlinear optics and IC order in condensed-matter systems

Towards a microscopic theory of toroidal moments in bulk periodic crystals

We present a theoretical analysis of magnetic toroidal moments in periodic systems, in the limit in which the toroidal moments are caused by a time and space reversal symmetry breaking arrangement of localized magnetic dipole moments. We summarize the basic definitions for finite systems and address the question of how to generalize these definitions to the bulk periodic case. We define the toroidization as the toroidal moment per unit cell volume, and we show that periodic boundary conditions lead to a multivaluedness of the toroidization, which suggests that only differences in toroidization are meaningful observable quantities. Our analysis bears strong analogy to the modern theory of electric polarization in bulk periodic systems, but we also point out some important differences between the two cases. We then discuss the instructive example of a one-dimensional chain of magnetic moments, and we show how to properly calculate changes of the toroidization for this system. Finally, we evaluate and discuss the toroidization (in the local dipole limit) of four important example materials: BaNiF_4, LiCoPO_4, GaFeO_3, and BiFeO_3.Comment: replaced with final (published) version, which includes some changes in the text to improve the clarity of presentatio

Terahertz and infrared spectroscopic evidence of phonon-paramagnon coupling in hexagonal piezomagnetic YMnO3

Terahertz and far-infrared electric and magnetic responses of hexagonal piezomagnetic YMnO3 single crystals are investigated. Antiferromagnetic resonance is observed in the spectra of magnetic permeability mu_a [H(omega) oriented within the hexagonal plane] below the Neel temperature T_N. This excitation softens from 41 to 32 cm-1 on heating and finally disappears above T_N. An additional weak and heavily-damped excitation is seen in the spectra of complex dielectric permittivity epsilon_c within the same frequency range. This excitation contributes to the dielectric spectra in both antiferromagnetic and paramagnetic phases. Its oscillator strength significantly increases on heating towards room temperature thus providing evidence of piezomagnetic or higher-order couplings to polar phonons. Other heavily-damped dielectric excitations are detected near 100 cm-1 in the paramagnetic phase in both epsilon_c and epsilon_a spectra and they exhibit similar temperature behavior. These excitations appearing in the frequency range of magnon branches well below polar phonons could remind electromagnons; however, their temperature dependence is quite different. We have used density functional theory for calculating phonon dispersion branches in the whole Brillouin zone. A detailed analysis of these results and of previously published magnon dispersion branches brought us to the conclusion that the observed absorption bands stem from phonon-phonon and phonon- paramagnon differential absorption processes. The latter is enabled by a strong short-range in-plane spin correlations in the paramagnetic phase.Comment: subm. to PR

A Theory of the Pseudogap State of the Cuprates

The phase diagram for a general model for Cuprates is derived in a mean-field approximation. A phase violating time-reversal without breaking translational symmetry is possible when both the ionic interactions and the local repulsions are large compared to the energy difference between the Cu and O single-particle levels. It ends at a quantum critical point as the hole or electron doping is increased. Such a phase is necessarily accompanied by singular forward scattering such that, in the stable phase, the density of states at the chemical potential, projected to a particular point group symmetry of the lattice is zero producing thereby an anisotropic gap in the single-particle spectrum. It is suggested that this phase occupies the "pseudogap" region of the phase diagram of the cuprates. The temperature dependence of the single-particle spectra, the density of states, the specific heat and the magnetic susceptibility are calculated with rather remarkable correspondence with the experimental results. The importance of further direct experimental verification of such a phase in resolving the principal issues in the theory of the Cuprate phenomena is pointed out. To this end, some predictions are provided.Comment: 41 pages, 8 figure

Advanced resistivity model for arbitrary magnetization orientation applied to a series of compressive- to tensile-strained (Ga,Mn)As layers

The longitudinal and transverse resistivities of differently strained (Ga,Mn)As layers are theoretically and experimentally studied as a function of the magnetization orientation. The strain in the series of (Ga,Mn)As layers is gradually varied from compressive to tensile using (In,Ga)As templates with different In concentrations. Analytical expressions for the resistivities are derived from a series expansion of the resistivity tensor with respect to the direction cosines of the magnetization. In order to quantitatively model the experimental data, terms up to the fourth order have to be included. The expressions derived are generally valid for any single-crystalline cubic and tetragonal ferromagnet and apply to arbitrary surface orientations and current directions. The model phenomenologically incorporates the longitudinal and transverse anisotropic magnetoresistance as well as the anomalous Hall effect. The resistivity parameters obtained from a comparison between experiment and theory are found to systematically vary with the strain in the layer.Comment: 14 pages, 11 figures, submitted to Phys. Rev.

Theory of Non-Reciprocal Optical Effects in Antiferromagnets: The Case Cr_2O_3

A microscopic model of non-reciprocal optical effects in antiferromagnets is developed by considering the case of Cr_2O_3 where such effects have been observed. These effects are due to a direct coupling between light and the antiferromagnetic order parameter. This coupling is mediated by the spin-orbit interaction and involves an interplay between the breaking of inversion symmetry due to the antiferromagnetic order parameter and the trigonal field contribution to the ligand field at the magnetic ion. We evaluate the matrix elements relevant for the non-reciprocal second harmonic generation and gyrotropic birefringence.Comment: accepted for publication in Phys. Rev.