The spin wave spectra of multiferroic BiFeO3 films is calculated using a phenomenological Landau theory that includes magnetostatic effects. The lowest frequency magnon dispersion is shown to be quite sensitive to the angle between spin wave propagation vector and the Neel moment. Since electrical switching of the Neel moment has recently been demonstrated in this material, the sensitivity of the magnon dispersion permits direct electrical switching of spin wave propagation. This effect can be used to construct spin wave logical gates without current pulses, potentially allowing reduced power dissipation per logical operation.
We report the spectra of magnetically induced electric dipole absorption in Eu$_{0.75}$Y$_{0.25}$MnO$_3$ from temperature dependent far infrared spectroscopy (10-250 cm$^{-1}$). These spectra, which occur only in the $e||a$ polarization, consist of two relatively narrow electromagnon features that onset at $T_{FE}=30$ K and a broad absorption band that persists to temperatures well above $T_N=47$ K. The observed excitations account for the step up of the static dielectric constant in the ferroelectric phase. The electromagnon at 80 cm$^{-1}$ is observed to be strongly coupled to the nearby low…
LuFe2O4 exhibits multiferroicity due to charge order on a frustrated triangular lattice. We find that the magnetization of LuFe2O4 in the multiferroic state can be electrically controlled by applying voltage pulses. Depending on with or without magnetic fields, the magnetization can be electrically switched up or down. We have excluded thermal heating effect and attributed this electrical control of magnetization to an intrinsic magnetoelectric coupling in response to the electrical breakdown of charge ordering. Our findings open up a new route toward electrical control of magnetization.
The breakdown of magnons, the quasiparticles of magnetic systems, has rarely been seen. By using an inelastic neutron scattering technique we report the observation of spontaneous magnon decay in multiferroic LuMnO$_3$, a simple two-dimensional Heisenberg triangular lattice antiferromagnet, with large spin, S = 2. The origin of this rare phenomenon lies in the non-vanishing cubic interaction between magnons in the spin Hamiltonian arising from the noncollinear 120$^o$ spin structure. We observed all three key features of the nonlinear effects as theoretically predicted: a roton-like minimum, a…
The magnon and optical phonon spectrum of an incommensurate multiferroic such as BiFeO3 is considered in the framework of a phenomenological Landau theory. The resulting spin wave spectrum is quite distinct from commensurate substances due to soft mode anisotropy and magnon zone folding. The former allows electrical control of spin wave propagation via reorientation of the spontaneous ferroelectric moment. The latter gives rise to multiple magneto-dielectric resonances due to the coupling of optical phonons at zero wavevector to magnons at integer multiples of the cycloid wavevector. These res…
We used Raman and terahertz spectroscopies to investigate lattice and magnetic excitations and their cross-coupling in the hexagonal YMnO3 multiferroic. Two phonon modes are strongly affected by the magnetic order. Magnon excitations have been identified thanks to comparison with neutron measurements and spin wave calculations but no electromagnon has been observed. In addition, we evidenced two additional Raman active peaks. We have compared this observation with the anti-crossing between magnon and acoustic phonon branches measured by neutron. These optical measurements underly the unusual s…
Inelastic neutron scattering has been used to study the magneto-elastic excitations in the multiferroic manganite hexagonal YMnO$_3$. An avoided crossing is found between magnon and phonon modes close to the Brillouin zone boundary in the $(a,b)$-plane. Neutron polarization analysis reveals that this mode has mixed magnon-phonon character. An external magnetic field along the $c$-axis is observed to cause a linear field-induced splitting of one of the spin wave branches. A theoretical description is performed, using a Heisenberg model of localized spins, acoustic phonon modes and a magneto-ela…
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 a…
We demonstrate a new approach for directly measuring the ultrafast energy transfer between elec- trons and magnons, enabling us to track spin dynamics in an antiferromagnet (AFM). In multiferroic HoMnO3, optical photoexcitation creates hot electrons, after which changes in the spin order are probed with a THz pulse tuned to a magnon resonance. This reveals a photoinduced transparency, which builds up over several picoseconds as the spins heat up due to energy transfer from hot elec- trons via phonons. This spin-lattice thermalization time is ?10 times faster than that of typical ferromagnetic …
Low-energy magnon excitations in multiferroic BiFeO$_3$ were measured in detail as a function of temperature around several Brillouin zone centers by inelastic neutron scattering experiments on single crystals. Unique features around 1 meV are directly associated with the interplay of the Dzyaloshinskii-Moriya interaction and a small single-ion anisotropy. The temperature dependence of these and the exchange interactions were determined by fitting the measured magnon dispersion with spin-wave calculations. The spectra best fits an easy-axis type magnetic anisotropy and the deduced exchange and…
We report electrical, magnetic, magnetodielectric and magnetoabsorption properties of a polycrystalline GaFeO3. The resistivity measurement shows that the sample is highly insulating below 200 K and the resistivity above 200 K obey the Arrhenius law with an activation energy of Ea = 0.67 eV. An anomaly occurs in the temperature dependence of permittivity (e) near the ferrimagnetic transition temperature (TC = 228 K) in a zero magnetic field and it is suppressed under H = 60 mT which indicates a possible magnetoelectric coupling in GaFeO3 with a fractional change of de/e = -1.8% at 60 mT around…
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 magnetic excitations in multiferroic TbMnO3 have been studied by inelastic neutron scattering in the spiral and sinusoidally ordered phases. At the incommensurate magnetic zone center of the spiral phase, we find three low-lying magnons whose character has been fully determined using neutron-polarization analysis. The excitation at the lowest energy is the sliding mode of the spiral, and two modes at 1.1 and 2.5meV correspond to rotations of the spiral rotation plane. These latter modes are expected to couple to the electric polarization. The 2.5meV-mode is in perfect agreement with recent…
Various phenomena related to inhomogeneous magnetoelectric interaction are considered. The interrelation between spatial modulation of order parameter and electric polarization, known as flexoelectric effect in liquid crystals, in the case of magnetic media appears in a form of electric polarization induced by spin modulation and vice versa. This flexomagnetoelectric interaction is also related to the influence of ferroelectric domain structure on antiferromagnetic vector distribution, and to the magnetoelectric properties of micromagnetic structures. The influence of inhomogeneous magnetoelec…
We present a theory of magnetoelectric magnon-photon coupling in cavities hosting noncentrosymmetric magnets. Analogously to nonreciprocal phenomena in multiferroics, the magnetoelectric coupling is time-reversal and inversion asymmetric. This asymmetry establishes a means for exceptional tunability of magnon-photon coupling, which can be switched on and off by reversing the magnetization direction. Taking the multiferroic skyrmion-host Cu$_2$OSeO$_3$ with ultralow magnetic damping as an example, we reveal the electrical activity of skyrmion eigenmodes and propose it for magnon-photon splittin…
Multiferroics are singular materials that can display simultaneously electric and magnetic orders. Some of them can be ferroelectric and ferromagnetic and, for example, provide the unique opportunity of encoding information independently in electric polarization and magnetization to obtain four different logic states. However, schemes allowing a simple electrical readout of these different states have not been demonstrated so far. In this article, we show that this can be achieved if a multiferroic material is used as the tunnel barrier in a magnetic tunnel junction. We demonstrate that thin f…
We report the structural and magnetoelectrical properties of La$_{0.7}$Ca$_{0.3}$MnO$_3$/BaTiO$_3$ perovskite superlattices grown on (001)-oriented SrTiO$_3$ by the pulsed laser deposition technique. Magnetic hysteresis loops together with temperature dependent magnetic properties exhibit well-defined coercivity and magnetic transition temperature (T$_C$) \symbol{126}140 K. $DC$ electrical studies of films show that the magnetoresistance (MR) is dependent on the BaTiO$_3$ thickness and negative $MR$ as high as 30% at 100K are observed. The $AC$ electrical studies reveal that the impedance and …
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 co…
Type-II multiferroic materials, in which ferroelectric polarization is induced by inversion non-symmetric magnetic order, promise new and highly efficient multifunctional applications based on the mutual control of magnetic and electric properties. Although this phenomenon has to date been limited to low temperatures, here we report a giant pressure-dependence of the multiferroic critical temperature in CuBr$_2$. At 4.5 GPa, $T_\mathrm{C}$ is enhanced from 73.5 to 162 K, to our knowledge the highest value yet reported for a non-oxide type-II multiferroic. This growth shows no sign of saturatin…
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…
We have directly imaged reversible electrical switching of the cycloidal rotation direction (magnetic polarity) in a (111)-BiFeO3 epitaxial-film device at room temperature by non-resonant x-ray magnetic scattering. Consistent with previous reports, fully relaxed (111)-BiFeO3 epitaxial films consisting of a single ferroelectric domain were found to comprise a sub-micron-scale mosaic of magneto-elastic domains, all sharing a common direction of the magnetic polarity, which was found to switch reversibly upon reversal of the ferroelectric polarization without any measurable change of the magneto-…
The electric field effect on magnetism was examined in the multiferroic conical magnet Mn$_2$GeO$_4$, which shows a strong coupling between ferromagnetic and ferroelectric order parameters. The systematic evaluation of the electric polarization in the multiferroic phase below 5.5 K under various field cooling conditions reveals that small magnetic fields of 0.1 T significantly reduce the required electric fields needed to reach saturation. By applying electric fields during magnetic field dependent hysteresis measurements of magnetization M and polarization P an electrically controllable excha…
We uncover a new pathway towards multiferroicity, showing how magnetism can drive ferroelectricity without relying on inversion symmetry breaking of the magnetic ordering. Our free-energy analysis demonstrates that any commensurate spin-density-wave ordering with a phase dislocation, even if it is collinear, gives rise to an electric polarization. Due to the dislocation the electronic and magnetic and inversion centers do not coincide, which turns out to be a sufficient condition for multiferroic coupling. The novel mechanism explains the formation of multiferroic phases at the magnetic commen…
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…
The symmetry conditions for the development of a macroscopic electrical polarization as a secondary order parameter to a magnetic ordering transition, and the constraints on the direction of the polarization vector, are determined by a non-conventional application of the theory of irreducible co-representations. In our approach, which is suitable for both magnetic and structural modulations, anti-unitary operators are employed to describe symmetry operations that exchange the propagation vector $\textbf{k}$ with $\textbf{-k}$, rather than operations combined with time-reversal as in classical …
Magnetic dc susceptibility between 1.5 and 800 K, ac susceptibility and magnetization, thermodynamic properties, temperature dependence of radio and audio-wave dielectric constants and conductivity, contact-free dielectric constants at mm-wavelengths, as well as ferroelectric polarization are reported for single crystalline BiFeO3. A well developed anomaly in the magnetic susceptibility signals the onset of antiferromagnetic order close to 635 K. Beside this anomaly no further indications of phase or glass transitions are indicated in the magnetic dc and ac susceptibilities down to the lowest …
We study the nonlinear magnon spin current induced by an ac electric field under light irradiation in collinear antiferromagnets with broken inversion symmetry. For linearly polarized light, we find that a dc spin current appears through ``the magnon spin shift current" mechanism, which is driven by a spin polarization generation in the two magnon creation process and has a close relationship to the geometry of magnon bands through Berry connection. For circularly polarized light, a dc spin current appears through ``the spin injection current" mechanism, which is proportional to the relaxation…
To understand the unexpectedly high thermoelectric performance observed in the thin-film Heusler alloy Fe$_2$V$_{0.8}$W$_{0.2}$Al, we study the magnon drag effect, generated by the tungsten based impurity band, as a possible source of this enhancement, in analogy to the phonon drag observed in FeSb$_2$. Assuming that the thin-film Heusler alloy has a conduction band integrating with the impurity band, originated by the tungsten substitution, we derive the electrical conductivity $L_{11}$ based on the self-consistent t-matrix approximation and the thermoelectric conductivity $L_{12}$ due to mag…
The idea of embedding and transmitting information within the fluctuations of the magnetic moments of spins (spin waves) has been recently proposed and experimentally tested. The coherence of spin waves, which describes how well defined these excitations are, is of course vital to this process, and themost significant factor that affects the spin-wave coherence is temperature. Here we present neutron inelastic scattering measurements of the full threedimensional spin-wave dispersion in BiFeO3, which is one of the most promising functional multiferroic material, for temperatures from 5K to 700K…
Magnetic order and excitations in multiferroic DyMnO3 were studied by neutron scattering experiments using a single crystal prepared with enriched 162Dy isotope. The ordering of Mn moments exhibits pronounced hysteresis arising from the interplay between Mn and Dy magnetism which possesses a strong impact on the ferroelectric polarization. The magnon dispersion resembles that reported for TbMnO3. We identify the excitations at the magnetic zone center and near the zone boundary in the b direction, which can possess electromagnon character. The lowest frequency of the zone-center magnons is in …
Some magnetoelectric multiferroics have a canted spin structure that can be described by a Dzyaloshinkii-Moriya coupling. We calculate properties and features expected for surface and bulk magnon polaritons in such media with a linear magnetoelectric interaction for the case of transverse electric polarisation. The dielectric polarisation and magnetisation of weak ferromagnetism are constrained to lie in the plane parallel to the surface. We examine a geometry with the polarisation oriented in the film plane and present numerical results for the transverse electric polarisation. Particular att…
Multiferroics, showing simultaneous ordering of electrical and magnetic degrees of freedom, are remarkable materials as seen from both the academic and technological points of view. A prominent mechanism of multiferroicity is the spin-driven ferroelectricity, often found in frustrated antiferromagnets with helical spin order. There, similar to conventional ferroelectrics, the electrical dipoles arise from an off-centre displacement of ions. However, recently a different mechanism, namely purely electronic ferroelectricity, where charge order breaks inversion symmetry, has attracted considerabl…
This paper reports on a theoretical proposal for electrical creation of magnetic skyrmions on a thin-film specimen of a multiferroic chiral magnet by local application of an electric field, instead of an electric current, via an electrode tip. This method can be traced back to the mutual coupling between skyrmion spins and the electric polarizations in multiferroics, and represents a unique technique for use in potential skyrmion-based memory devices without Joule-heating losses.
We present an investigation of the multiferroic lacunar spinel compound GeV$_4$S$_8$ using time-domain terahertz spectroscopy. We find three absorptions which either appear or shift at the antiferromagnetic transition temperature, T$_N = 17$ K, as S=1 magnetic moments develop on vanadium tetrahedra. Two of these absorptions are coupled to the magnetic state and one only appears below the Néel temperature, and is interpreted as a magnon. We also observe isosbestic points in the dielectric constant in both the temperature and frequency domains. Further, we perform analysis on the isosbestic feat…
We studied spin excitations of the multiferroic Ba2CoGe2O7 in high magnetic fields up to 33 T. In the electron spin resonance and far infrared absorption spectra we found several spin excitations beyond the two conventional magnon modes expected for such a two-sublattice antiferromagnet. We show that a multi-boson spin-wave theory can capture these unconventional modes, that include spin-stretching modes associated with an oscillating magnetic dipole (or only quadrupole) moment. The lack of the inversion symmetry allows these modes to become electric dipole active. We expect that the spin-stre…
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.
Lattice and spin excitations have been studied by Raman scattering in hexagonal YbMnO3 single crystals. The temperature dependences of the phonon modes show that the E2 mode at 256 cm-1 related to the displacement of Mn and O ions in a-b plane is coupled to the spin order. The A1 phonon mode at 678 cm-1 presents a soft mode behavior at the Neel temperature. Connected to the motion of the apical oxygen ions along the c direction, this mode controls directly the Mn-Mn interactions between adjacent Mn planes and the superexchange path. Crystal field and magnon mode excitations have been identifie…
We theoretically discover that unique eigenmodes of skyrmion crystal (SkX) are not only magnetically active to ac magnetic field (H^w) but also electrically active to ac electric field (E^w) in a multiferroic chiral-lattice magnet Cu2OSeO3, which amplifies the dynamical magnetoelectric coupling between E^w and the spin texture. The resulting intense interference between their electric and magnetic activation processes can lead to unprecedentedly large diode effect on the microwave, i.e., its absorption by SkX changes up to ~20% when the incident direction is reversed. Our results demonstrate t…
The low energy dynamical properties of the multiferroic hexagonal perovskite ErMnO3 have been studied by inelastic neutron scattering as well as terahertz and far infrared spectroscopies on synchrotron source. From these complementary techniques, we have determined the magnon and crystal field spectra and identified a zone center magnon only excitable by the electric field of an electromagnetic wave. Using comparison with the isostructural YMnO3 compound and crystal field calculations, we propose that this dynamical magnetoelectric process is due to the hybridization of a magnon with an electr…
Spin excitations were studied by absorption spectroscopy in CaBaCo4O7 which is a type-I multiferroic compound with the largest magnetic-order induced ferroelectric polarization (ΔP=17mC/m2) reported, so far. We observed two optical magnon branches: a solely electric dipole allowed one and a mixed magnetoelectric resonance. The entangled magnetization and polarization dynamics of the magnetoelectric resonance gives rise to unidirectional light absorption, i.e. that magnon mode absorbs the electromagnetic radiation for one propagation direction but not for the opposite direction. Our systematic …
We report on the different roles of two orbital-active Fe$^{2+}$ at the A site and V$^{3+}$ at the B site in the magnetic excitations and on the anomalous spin wave broadening in FeV$_{2}$O$_{4}$. FeV$_{2}$O$_{4}$ exhibits three structural transitions and successive paramagnetic (PM)-collinear ferrimagnetic (CFI)-noncollinear ferrimagnetic (NCFI) transitions. The high-temperature tetragonal/PM -orthorhombic/CFI transition is accompanied by the appearance of an energy gap with a high magnitude in the magnetic excitations due to strong spin-orbit coupling induced anisotropy at the Fe$^{2+}$ site…
