Coupled Spin-Phonon Excitations in Helical Multiferroics

Both the Dzyaloshiskii-Moriya interaction and the exchange-striction are shown to affect dynamically the magnetoelectric excitations in the perovskite multiferroic RMnO3. The exchange-striction results in a biquadratic interaction between the spins and the transverse phonons, giving rise to quantum fluctuations of the ferroelectric polarization P. This leads to low-lying phonon modes that are perpendicular to P and to the helical spins at small wave vector but are parallel to P at a wave vector close to the magnetic modulation vector. For spin-1/2 helimagnet, the local polarization can be completely reversed by the spin fluctuation, and so does the direction of the on-site spin chirality, which allows for a finite differential scattering intensity of polarized neutrons from a cycloidal magnet.Comment: 7 page

Internal magnetic field effect on magnetoelectricity in orthorhombic RMnO3RMnO_3 crystals

We have investigated the role of the 4$f$ moment on the magnetoelectric (ME) effect of orthorhombic $R$MnO$_{3}$ ($R$=rare earth ions). In order to clarify the role of the 4$f$ moment, we prepared three samples: (Eu,Y)MnO$_{3}$ without the 4$f$ moment, TbMnO$_{3}$ with the anisotropic 4$f$ moment, and (Gd,Y)MnO$_{3}$ with the isotropic 4$f$ moment. The ferroelectric behaviors of these samples are different from each other in a zero magnetic field. (Eu,Y)MnO$_{3}$ and (Gd,Y)MnO$_{3}$ show the ferroelectric polarization along the a axis in the ground state, while TbMnO$_{3}$ shows it along the c axis. Such difference may arise from the influence of the anisotropic Tb$^{3+}$ 4$f$ moment. The direction of the ferroelectric polarization of $R$MnO$_{3}$ is determined by the internal magnetic field arising from the 4$f$ moment.Comment: 2 pages, 1 figure, the proceeding of International Conference of Magnetism, to be published in the Journal of Magnetism and Magnetic Material

Electric-dipole active two-magnon excitation in {\textit{ab}} spiral spin phase of a ferroelectric magnet Gd0.7_{\textbf{0.7}}Tb0.3_{\textbf{0.3}}MnO3_{\textbf 3}

A broad continuum-like spin excitation (1--10 meV) with a peak structure around 2.4 meV has been observed in the ferroelectric $ab$ spiral spin phase of Gd$_{0.7}$Tb$_{0.3}$MnO$_3$ by using terahertz (THz) time-domain spectroscopy. Based on a complete set of light-polarization measurements, we identify the spin excitation active for the light $E$ vector only along the a-axis, which grows in intensity with lowering temperature even from above the magnetic ordering temperature but disappears upon the transition to the $A$-type antiferromagnetic phase. Such an electric-dipole active spin excitation as observed at THz frequencies can be ascribed to the two-magnon excitation in terms of the unique polarization selection rule in a variety of the magnetically ordered phases.Comment: 11 pages including 3 figure

Mechanism of Lattice-Distortion-Induced Electric-Polarization Flop in the Multiferroic Perovskite Manganites

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.Comment: 5 pages, 5 figures. Recalculated results after correcting errors in the assignment of DM vectors. The conclusion is not affecte

Spin chirality and electric polarization in multiferroic compounds RRMn2_2O5_5 (R=R=Ho, Er)

Polarized neutron diffraction experiments have been performed on multiferroic materials $R$Mn$_{2}$O$_{5}$ ($R=$Ho, Er) under electric fields in the ferroelectric commensurate (CM) and the low-temperature incommensurate (LT-ICM) phases, where the former has the highest electric polarization and the latter has reduced polarization. It is found that, after cooling in electric fields down to the CM phase, the magnetic chirality is proportional to the electric polarization. Also we confirmed that the magnetic chirality can be switched by the polarity of the electric polarization in both the CM and LT-ICM phases. These facts suggest an intimate coupling between the magnetic chirality and the electric polarization. However, upon the transition from the CM to LT-ICM phase, the reduction of the electric polarization is not accompanied by any reduction of the magnetic chirality, implying that the CM and LT-ICM phases contain different mechanisms of the magnetoelectric coupling.Comment: 4 pages, 2 figures. Proceedings of PNCMI2008/QuBS200

Roles of Bond Alternation in Magnetic Phase Diagram of RMnO3

In order to investigate nature of the antiferromagnetic structures in perovskite RMnO3, we study a Heisenberg J1-J2 model with bond alternation using analytical and numerical approaches. The magnetic phase diagram which includes incommensurate spiral states and commensurate collinear states is reproduced. We discuss that the magnetic structure with up-up-down-down spin configuration (E-type structure) and the ferroelectricity emerge cooperatively to stabilize this phase. Magnetoelastic couplings are crucial to understand the magnetic and electric phase diagram of RMnO3.Comment: 5 pages, 6 figure

Flexomagnetoelectric effect in bismuth ferrite

There is a profound analogy between inhomogeneous magnetoelectric effect in multiferroics and flexoelectric effect in liquid crystals. This similarity gives rise to the flexomagnetoelectric polarization induced by spin modulation. The theoretical estimations of flexomagnetoelectric polarization agree with the value of jumps of polarization in magnetoelectric dependences (~20muC/m^2) observed at spin cycloid suppression at critical magnetic field 200kOe.Comment: 6 pages,2 figure

CuBr2-A New Multiferroic Material with High Critical Temperature

A new multiferroic material, CuBr2, is reported for the first time. CuBr2 has not only a high transition temperature (close to liquid nitrogen temperature) but also low dielectric loss and strong magnetoelectric coupling. These findings reveal the importance of anion effects in the search for the high temperature multiferroics materials among these low-dimensional spin systems.Comment: 3 figures, accepted by Advanced Material

Anomalous Coexistence of Ferroelectric Phases (P∥aP\parallel a and P∥cP\parallel c) in Orthorhombic Eu1−y_{1-y}Yy_yMnO3_3 (y>0.5y>0.5) Crystals

We have investigated the magnetic and dielectric properties of orthorhombic Eu$_{1-y}$Y$_y$MnO$_3$ ($0\leq y\leq 0.6$) single crystals without the presence of the 4$f$ magnetic moments of the rare-earth ions. In $y\geq 0.2$, the magnetic-structure driven ferroelectricity is observed. The ferroelectric transition temperature is steeply reducing with increasing $y$. In $y\geq 0.52$, two ferroelectric phases ($P\parallel a$ and $P\parallel c$) are coexistent at low temperatures. In these phases, ferroelectricity has different origin, which is evidenced by the distinctive poling-electric-field dependence of electric polarization. Namely, the electric polarization along the c axis ($P_c$) is easily saturated by a poling electric field, therefore $P_c$ is caused by the $bc$ spiral antiferromagnetic order. On the other hand, the electric polarization along the a axis ($P_a$) is probably attributed to the collinear $E$-type antiferromagnetic order, because $P_a$ is unsaturated even in a poling field of $10^6$ V/m.Comment: 10 pages, 4figures, to be published in Journal of the Physical Society of Japa

Theory of magnetoelectric resonance in two-dimensional S=3/2S=3/2 antiferromagnet Ba2CoGe2O7{\rm Ba_2CoGe_2O_7} via spin-dependent metal-ligand hybridization mechanism

We investigate magnetic excitations in an $S=3/2$ Heisenberg model representing two-dimensional antiferromagnet ${\rm Ba_2CoGe_2O_7}$. In terahertz absorption experiment of the compound, Goldstone mode as well as novel magnetic excitations, conventional magnetic resonance at 2 meV and both electric- and magnetic-active excitation at 4 meV, have been observed. By introducing a hard uniaxial anisotropy term $\Lambda (S^z)^2$, three modes can be explained naturally. We also indicate that, via the spin-dependent metal-ligand hybridization mechanism, the 4 meV excitation is an electric-active mode through the coupling between spin and electric-dipole. Moreover, at 4 meV excitation, an interference between magnetic and electric responses emerges as a cross correlated effect. Such cross correlation effects explain the non-reciprocal linear directional dichroism observed in ${\rm Ba_2CoGe_2O_7}$.Comment: 5 pages, 3 figure