We have investigated electrically-active magnetic excitations (electromagnons) in perovskite manganites with the $E$-type (up-up-down-down) spin structure by terahertz spectroscopy. Eu$_{1-x}$Y$_x$MnO$_3$ (0.1$\le x\le$1) and Y$_{1-y}$Lu$_y$MnO$_3$ (0$\le y\le$1) without magnetic $f$-moments, which host collinear sinusoidal, $A$-type, cycloidal, and $E$-type spin orders, are used to examine the systematics of possible electromagnons. Three-peak structures (23, 35, 45 cm$^{-1}$) of magnetic origin show up in the $E$-type phase with little composition ($y$) dependence of frequencies, making a contrast with the electromagnons observed in the cycloidal-spin ($x\le0.8$) phases. One of these electromagnon is ascribed to the zone-edge magnon mode based on the calculated magnon dispersions.
All-electrical control of a dynamic magnetoelectric effect is demonstrated in a classical multiferroic manganite DyMnO3, a material containing coupled antiferromagnetic and ferroelectric orders. Due to intrinsic magnetoelectric coupling with electromagnons a linearly polarized terahertz light rotates upon passing through the sample. The amplitude and the direction of the polarization rotation are defined by the orientation of ferroelectric domains and can be switched by static voltage. These experiments allow the terahertz polarization to be tuned using the dynamic magnetoelectric effect.
We have investigated the time dependence of remanent magnetostriction in a (La,Pr)$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$ single crystal, in order to examine the slow dynamics of lattice distortion in bilayered manganites. A competition between double exchange and Jahn-Teller type orbital-lattice interactions results in the observed lattice profile following a stretched exponential function. This finding suggests that spatial growth of the local lattice distortions coupled with e$_{g}$-electron orbital strongly correlates with the appearance of the field-induced CMR effect.
Terahertz time-domain spectroscopy was performed to directly probe the low-energy (1-5 meV) electrodynamics of triangular lattice antiferromagnets CuFe1-xGaxO2 (x = 0.00, 0.01, and 0.035). We discovered an electromagnon (electric-field-active magnon) excitation at 2.3 meV in the paraelectric up-up-down-down collinear magnetic phase, while this electromagnon vanishes in the ferroelectric helimagnetic phase. Anti-correlation with noncollinear magnetism excludes the exchange-striction mechanism as the origin of dynamical magnetoelectric coupling, and hence evidences the observation of spin-orbit …
The behavior of the low-frequency electromagnon in multiferroic DyMnO3 has been investigated in external magnetic fields and in a magnetically ordered state. Significant softening of the electromagnon frequency is observed for external magnetic fields parallel to the a-axis (BIIa), revealing a number of similarities to a classical soft mode behavior known for ferroelectric phase transitions. The softening of the electromagnon yields an increase of the static dielectric permittivity which follows a similar dependence as predicted by the Lyddane-Sachs-Teller relation. Within the geometry BIIb th…
Magnetodielectric materials are characterized by a strong coupling of magnetic and dielectric properties and in rare cases simultaneously exhibit both, magnetic and polar order. Among other multiferroics, TbMnO3 and GdMnO3 reveal a strong magneto-dielectric (ME) coupling and as a consequence fundamentally new spin excitations exist: Electro-active magnons, or electromagnons, i. e. spin waves which can be excited by ac electric fields. Here we show that these excitations appear in the phase with an incommensurate (IC) magnetic structure of the manganese spins. In external magnetic fields this I…
Effects of temperature (6--225 K) and magnetic field (0--7 T) on the low-energy (1.2--5 meV) electrodynamics of the electromagnon, the magnetic resonance driven by the light electric field, have been investigated for a hexaferrite magnet Ba$_2$Mg$_2$Fe$_{12}$O$_{22}$ by using terahertz time-domain spectroscopy. We find the gigantic terahertz magnetochromism via electromagnons; the magnetochromic change, as defined by the difference of the absorption intensity with and without magnetic field, exceeds 500% even at 0.6 T. The results arise from the fact that the spectral intensity of the electrom…
We have studied the pressure effect on magnetostriction, both in the $ab$-plane and along the c-axis, of a (La,Pr)$_{1.2}$Sr$_{1.8}$Mn$_{2}$O$_{7}$ bilayered manganite single crystal over the temperature region where the field-induced ferromagnetic metal (FMM) transition takes place. For comparison, we have also examined the pressure dependence of magnetization curves at the corresponding temperatures. The applied pressure reduces the critical field of the FMM transition and it enhances the remanent magnetostriction. An anomalous pressure effect on the remanent lattice relaxation is observed a…
Complete magnetoelectric (ME) phase diagrams of orthorhombic $R$MnO$_{3}$ with and without magnetic moments on the $R$ ions have been established. Three kinds of multiferroic ground states, the $ab$-cycloidal, the $bc$-cycloidal, and the collinear $E$-type phases, have been identified by the distinct ME responses. The electric polarization of the $E$-type phase dominated by the symmetric spin exchange ($bm{S}_{i} cdot bm{S}_{j}$) is more than 10 times as large as that of the $bc$-cycloidal phase dominated by the antisymmetric one ($bm{S}_{i} times bm{S}_{j}$), and the ME response is enhanced n…
We show that strong electromagnon peaks can be found in absorption spectra of non-collinear magnets exhibiting a linear magnetoelectric effect. The frequencies of these peaks coincide with the frequencies of antiferromagnetic resonances and the ratio of the spectral weights of the electromagnon and antiferromagnetic resonance is related to the ratio of the static magnetoelectric constant and magnetic susceptibility. Using a Kagome lattice antiferromagnet as an example, we show that frustration of spin ordering gives rise to magnetoelastic instabilities at strong spin-lattice coupling, which tr…
The origin of electromagnon excitations in cycloidal \textit{R}MnO$_3$ is explained in terms of the Heisenberg coupling between spins despite the fact that the static polarization arises from the much weaker Dzyaloshinskii-Moriya (DM) exchange interaction. We present a model that incorporates structural characteristics of this family of manganites that is confirmed by far infrared transmission data as a function of temperature and magnetic field and inelastic neutron scattering results. A deep connection is found between the magnetoelectric dynamics of the spiral phase and the static magnetoel…
Recent spectroscopic studies at terahertz frequencies for a variety of multiferroics endowed with both ferroelectric and magnetic orders have revealed the possible emergence of a new collective excitation, frequently referred to as electromagnon. It is magnetic origin, but becomes active in response to the electric field component of light. Here we give an overview on our recent advance in the terahertz time-domain spectroscopy of electromagnons or electric-dipole active magnetic resonances, focused on perovskite manganites--$R$MnO$_3$ ($R$ denotes rare-earth ions). The respective electric and…
Terahertz magnetic resonance driven by the light electric field, now referred to as electromagnon, has stimulated interest due to its strong candidate for future spin-electronics. One unique characteristic of electromagnons is the terahertz magnetochromism, a color change by external magnetic field, as recently demonstrated in the hexaferrite. By taking perovskite manganites and hexaferrite as model cases, the current understating of the electromagnon activity is discussed in terms of the symmetric exchange mechanism.
The optical spectra in the family of multiferroic manganites RMnO3 is a great puzzle. Current models can not explain the fact that two strong electromagnons are present in the non-collinear spin cycloidal phase, with only one electromagnon surviving the transition into the collinear spin sinusoidal phase. We show that this is a signature of the presence of anomalous magnetoelectric coupling that breaks rotational invariance in spin space and generates oscillatory polarization in the ground state.
The magnetoelectric coupling, i.e., cross-correlation between electric and magnetic orders, is a very desirable property to combine functionalities of materials for next-generation switchable devices. Multiferroics with spin-driven ferroelectricity presents such a mutual interaction concomitant with magneto- and electro-active excitations called electromagnons. TbMnO3 is a paradigmatic material in which two electromagnons have been observed in the cycloidal magnetic phase. However, their observation in TbMnO3 is restricted to the cycloidal spin phase and magnetic ground states that can support…
We summarize the existing experimental data on electromagnons in multiferroic RMn2O5 compounds, where R denotes a rare earth ion, Y or Bi, and discuss a realistic microscopic model of these materials based on assumption that the microscopic mechanism of magnetically-induced ferroelectricity and electromagnon absorption relies entirely on the isotropic Heisenberg exchange and magnetostrictive coupling of spins to a polar lattice mode and does not involve relativistic effects. This model explains many magnetic and optical properties of RMn2O5 manganites, such as the spin re-orientation transitio…
Chirality, i.e., the right- and left-handedness of structure, is one of the key concepts in many fields of science including biology, chemistry and physics, and its manipulation is an issue of vital importance. The electron spins in solids can form chiral configurations. In perovskite manganites RMnO3 (R=Tb, Dy,...etc), the Mn-spins form a cycloidal structure, which induces ferroelectric polarization (P) through the relativistic spin-orbit interaction. This magnetism-induced ferroelectricity (multiferroics) and associated infrared-active spin waves (electromagnons) open a promising route to co…
Here we present a detailed study of the THz and FIR response of the mixed perovskite manganite system Eu$_{1-x}$Ho$_x$MnO$_3$ for holmium concentrations x = 0.1 and 0.3. We compare the magnetic excitations of the four different magnetically ordered phases (A-type antiferromagnetic, sinusoidally modulated collinear, helical phases with spin planes perpendicular to the crystallographic a and c axes). The transition between the two latter phases goes hand in hand with a switching of the ferroelectric polarization from P||a to P||c. Special emphasis is paid to the temperature dependence of the exc…
In contrast to well studied multiferroic manganites with a spiral structure, the electric polarization in multiferroic borates is induced within collinear antiferromagnetic structure and can easily be switched by small static fields. Because of specific symmetry conditions, static and dynamic properties in borates are directly connected, which leads to giant magnetoelectric and magnetodielectric effects. Here we prove experimentally that the giant magnetodielectric effect in samarium ferroborate SmFe3(BO3)4 is of intrinsic origin and is caused by an unusually large electromagnon situated in th…
We have investigated dielectric properties in Mott insulators GdMnO$_{3}$ and TbMnO$_{3}$ under magnetic fields and external quasihydrostatic pressures. In the case of GdMnO$_{3}$, thermal hysteresis for dielectric constant $ε$ and discontinuous lattice distortion were observed at ferroelectric transition temperature ($T_{C}$), and ferroelectric spontaneous polarization was suppressed by application of external pressure. These results indicate that the ferroelectric transition in GdMnO$_{3}$ is a first-order displacive-type one. On the other hand, the thermal hysteresis and discontinuous latti…
We have investigated dielectric properties in a series of crystals of $R$MnO$_{3}$ ($R$ is a rare earth ion) under magnetic fields and quasihydrostatic pressure. We have found that ferroelectric phase appeared in GdMnO$_3$ crystal below 13K. We have confirmed that a small spontaneous polarization exists along a axis ($P_a$) in the orthorhombic $Pbnm$ setting and that $P_a$ can be reversed by the dc electric field. The dielectric anomaly due to the ferroelectric transition accompanied thermal hysteresis and lattice striction. The ferroelectric transition temperature decreased with quasihydrosta…
We report an unusual giant linear magnetostrictive effect in the ferrimagnet Gd$_{2/3}$Ca$_{1/3}$MnO$_3$ ($T_{c} \approx$80 K). Remarkably, the magnetostriction, negative at high temperature ($T \approx T_{c}$), becomes positive below 15 K when the magnetization of the Gd sublattice overcomes the magnetization of the Mn sublattice. A rather simple model where the magnetic energy competes against the elastic energy gives a good account of the observed results and confirms that Gd plays a crucial role in this unusual observation. Unlike previous works in manganites where only striction associate…
We propose a new mechanism to induce a novel one-magnon excitation by the electric component of light in cycloidal spin states, i.e. so called electromagnon process. We calculated optical spectra in the cycloidal spin structures as observed in multiferroic perovskite manganites RMnO3 where novel magnetic excitations induced by oscillating electric fields are observed. When symmetric spin-dependent electric polarizations are introduced, we have light absorptions at terahertz frequencies with one- and two-magnon excitations driven by the electric component of light. Our results show that some pa…
Magnetic rare earths R have been proven to have a significant effect on the multiferroic properties of the orthorhombic manganites RMnO3. A re-examination of previous results from synchrotron based x-ray scattering experiments suggests that symmetric exchange striction between neighboring R and Mn ions may account for the enhancement of the ferroelectric polarization in DyMnO3 as well as the magnetic-field induced ferroelectricity in GdMnO3. In general, adding a second magnetic species to a multiferroic material may be a route to enhance its ferroelectric properties.
