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 excitations at this transition. We find a significant change of intensity indicating that the exchange striction mechanism cannot be the only mechanism to induce dipolar weight to spin-wave excitations. We also focus on excitations within the incommensurate collinear antiferromagnetic phase and find a so far unobserved excitation close to 40 cm$^{-1}$. A detailed analysis of optical weight gives a further unexpected result: In the multiferroic phase with P||c all the spectral weight of the electromagnons comes from the lowest phonon mode. However, for the phase with the polarization P||a additional spectral weight must be transferred from higher frequencies.
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…
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…
Inelastic x-ray scattering with meV energy resolution (IXS) is an ideal tool to measure collective excitations in solids and liquids. In non-resonant scattering condition, the cross section is strongly dominated by lattice vibrations (phonons). However, it is possible to probe additional degrees of freedom such as magnetic fluctuations that are strongly coupled to the phonons. The IXS spectrum of the coupled system will contain not only the phonon dispersion (majority component) but also the so far undetected magnetic correlation function (minority component). Here we report the discovery of s…
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…
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…
We propose a model for the pair of electromagnon excitations observed in the class of multiferroic materials {\it R}MnO$_3$ ({\it R} is a rare-earth ion). The model is based on a harmonic cycloid ground state interacting with a zone-edge magnon and its twin excitation separated in momentum space by two times the cycloid wave vector. The pair of electromagnons is activated by cross coupling between magnetostriction and spin-orbit interactions. Remarkably, the spectral weight of the twin electromagnon is directly related to the presence of a magnetically induced oscillatory polarization in the g…
We have investigated spin-wave excitations in a four-sublattice (4SL) magnetic ground state of a frustrated magnet CuFeO2, in which `electromagnon' (electric-field-active magnon) excitation has been discovered by recent terahertz time-domain spectroscopy [Seki et al. Phys. Rev. Lett. 105 097207 (2010)]. In previous study, we have identified two spin-wave branches in the 4SL phase by means of inelastic neutron scattering measurements under applied uniaxial pressure. [T. Nakajima et al. J. Phys. Soc. Jpn. 80 014714 (2011) ] In the present study, we have performed high-energy-resolution inelastic…
Magnetic excitations are investigated for a hexagonal polar magnet Fe2Mo3O8 by terahertz spectroscopy. We observed magnon modes including an electric-field active magnon, electromagnon, in the collinear antiferromagnetic phase with spins parallel to the c axis. We unravel the nature of these excitations by investigating the correlation between the evolution of the mode profile and the magnetic transition from antiferromagnetic to ferrimagnetic order induced by magnetic field or Zn-doping. We propose that the observed electromagnon mode involves the collective precession of the spins with oscil…
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 …
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 studied magnetic excitations in a low-temperature ferroelectric phase of the multiferroic YMn2O5 using inelastic neutron scattering (INS). We identify low-energy magnon modes and establish a correspondence between the magnon peaks observed by INS and electromagnon peaks observed in optical absorption [1]. Furthermore, we explain the microscopic mechanism, which results in the lowest-energy electromagnon peak, by comparing the inelastic neutron spectral weight with the polarization in the commensurate ferroelectric phase.
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…
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 excitati…
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 infrared and Terahertz properties of GdMnO_3 have been investigated as function of temperature and magnetic field, with special emphasis on the phase boundary between the incommensurate and the canted antiferromagnetic structures. The heterogeneous incommensurate phase reveals strong magnetodielectric effects, characterized by significant magnetoelectric contributions to the static dielectric permittivity and by the existence of electrically excited magnons (electromagnons). In the commensurate canted antiferromagnetic phase the magnetoelectric contributions to the dielectric constant and …
The phenomenological theory of ferroelectricity in spiral magnets presented in [M. Mostovoy, Phys. Rev. Lett. 96, 067601 (2006)] is generalized to describe consistently states with both uniform and modulated-in-space ferroelectric polarizations. A key point in this description is the symmetric part of the magnetoelectric coupling since, although being irrelevant for the uniform component, it plays an essential role for the non-uniform part of the polarization. We illustrate this importance in generic examples of modulated magnetic systems: longitudinal and transverse spin-density wave states a…
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…
Understanding ultrafast magnetization dynamics on the microscopic level is of strong current interest due to the potential for applications in information storage. In recent years, the spin-lattice coupling has been recognized to be essential for ultrafast magnetization dynamics. Magnetoelectric multiferroics of type II possess intrinsic correlations among magnetic sublattices and electric polarization (P) through spin-lattice coupling, enabling fundamentally coupled dynamics between spins and lattice. Here we report on ultrafast magnetization dynamics in a room-temperature multiferroic hexafe…
Recently, oxide multiferroics have attracted much attention due to their large magnetoelectric effect which allows the tuning of magnetic properties with electric field and vice versa and open new venues for future spintronic applications such as multiple-state memory devices with dual magnetic and electric control. BiFeO$_3$ (BFO) belongs to this new class of materials and shows both ferroelectric and antiferromagnetic orders at room temperature with a large electric polarizationassociated with a cycloidal spiral magnetic ordering. The incommensurate magnetic order induces magnon zone folding…
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…
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…
The magnetic correlations in the charge- and orbital-ordered manganite La(0.5)Sr(1.5)MnO(4) have been studied by elastic and inelastic neutron scattering techniques. Out of the well-defined CE-type magnetic structure with the corresponding magnons a competition between CE-type and ferromagnetic fluctuations develops. Whereas ferromagnetic correlations are fully suppressed by the static CE-type order at low temperature, elastic and inelastic CE-type correlations disappear with the melting of the charge-orbital order at high temperature. In its charge-orbital disordered phase, La(0.5)Sr(1.5)MnO(…
Spin excitations of magnetoelectric LiNiPO$_4$ are studied by infrared absorption spectroscopy in the THz spectral range as a function of magnetic field through various commensurate and incommensurate magnetically ordered phases up to 33\,T. Six spin resonances and a strong two-magnon continuum are observed in zero magnetic field. Our systematic polarization study reveals that some of the excitations are usual magnetic-dipole active magnon modes, while others are either electromagnons, electric-dipole active, or magnetoelectric, both electric- and magnetic-dipole active spin excitations. Field…
Competing magnetic exchange interactions often result in non-collinear magnetic states, such as spin spirals, which break the inversion symmetry and induce ferroelectric polarization. The resulting strong interactions between magnetic and dielectric degrees of freedom lead to a technologically important possibility to control magnetic order by electric fields and to electromagnons, magnetic excitations that can be excited by an electric dipole of the electromagnetic field. Here we study the effects of chiral domain walls on magnetoelectric properties of spiral magnets. We use a quasi-1D model …
The magnon dispersion in the charge, orbital and spin ordered phase in La(0.5)Sr(1.5)MnO(4) has been studied by means of inelastic neutron scattering. We find an excellent agreement with a magnetic interaction model basing on the CE-type superstructure. The magnetic excitations are dominated by ferromagnetic exchange parameters revealing a nearly-one dimensional character at high energies. The nearest neighbor ferromagnetic interaction in La(0.5)Sr(1.5)MnO(4) is significantly larger than the one in the metallic ferromagnetically ordered manganites. The large ferromagnetic interaction in the ch…
We have studied the spin dynamics in Pr$_{0.63}$Sr$_{0.37}$MnO$_3$ above and below the Curie temperature $T_C=301$ K. Three distinct new features have been observed: a softening of the magnon dispersion at the zone boundary for $T<T_C$, significant broadening of the zone boundary magnons as $T\to T_C$, and no evidence for residual spin-wave like excitations just above $T_C$. The results are inconsistent with double exchange models that have been successfully applied to higher $T_C$ samples, indicating an evolution of the spin system with decreasing $T_C$.
We investigate magnetic excitations in half-doped colossal magnetoresistance manganites. In particular, we focus on spin excitations in the CE phase originally proposed by Goodenough (Phys. Rev. 100, 564 (1955)). Using a localized spin model we calculated magnons for 3D-perovskite compounds such as La$_{1-x}$M$_x$MnO$_3$, where M=Ca,Sr,Ba, and for their 2D-laminar counterparts. We compared them with predictions for the spin excitations corresponding to other phases proposed. For the laminar half-doped manganite La$_{0.5}$Sr$_{1.5}$MnO$_4$, for which magnon measurements by inelastic neutron sca…
Inelastic neutron scattering experiments have been performed on single crystals of Nd$_{1-x}$Sr$_{x}$MnO$_{3}$ with x$\approx$0.5. Colossal magnetoresistance (CMR) in the manganites arises from the interplay between a ferromagnetic metallic and antiferromagnetic charge and orbital ordered insulating state. Therefore, it appears important to compare these phases concerning their underlying magnetic interaction parameters. Our investigations of the spin-wave disperion in the AFM ordered state of Nd$_{0.5}$Sr$_{0.5}$MnO$_{3}$ exhibits a strongly anisotropic stiffness. The sign of the anisotropy i…
Collapse of Jahn-Teller Phonons in La$_{1-x}$Sr$_{x}$MnO$_3$ with Weak Magnetoresistance
University of Colorado Boulder（科罗拉多大学博尔德分校）；Oak Ridge National Laboratory（橡树岭国家实验室）；Japan Atomic Energy Agency（日本原子能机构）；High Energy Accelerator Research Organization (KEK)（高能加速器研究机构）；Comprehensive Research Organization for Science and Society（综合科学研究组织）；Karlsruhe Institute of Technology（卡尔斯鲁厄理工学院）
We investigated the spin excitations of magnetoelectric $\text{LiFePO}_4$ by THz absorption spectroscopy in magnetic fields up to 33$\,$T. By studying their selection rules, we found not only magnetic-dipole, but also electric-dipole active (electromagnons) and magnetoelectric resonances. The magnetic field dependence of four strong low-energy modes is reproduced well by our four-sublattice spin model for fields applied along the three orthorhombic axes. From the fit, we refined the exchange couplings, single-ion anisotropies, and the Dzyaloshinskii-Moriya interaction parameters. Additional sp…
Oxygen-isotope effects on the intrinsic resistivity have been studied in high-quality epitaxial thin films of La_{0.75}Ca_{0.25}MnO_{3} and Nd_{0.7}Sr_{0.3}MnO_{3}. We found that the residual resistivity ρ_{o} increases by about 15(3)% upon replacing ^{16}O by ^{18}O. This provides strong evidence for the presence of small or intermediate-size polarons in the metallic ferromagnetic state. Furthermore, the temperature dependent part of the resistivity at low temperatures consists of an AT^{4.5} term contributed from 2-magnon scattering, and a Bω_{s}/\sinh^{2}(\hbarω_{s}/2k_{B}T) term which aris…
At half doping, the ground state of three-dimensional manganite perovskite oxides like R$_{1-x}$Ca$_x$MnO$_3$, where R is a trivalent ion such as La, Pr, etc, is still unclear. Many experimental findings agree better with the combined magnetic, charge, and orbital order characteristic of the "intermediate phase", introduced by Efremov et al. in 2004 [Nature Mats. 3, 853]. This phase consists of spin dimers (thus incorporating aspects of the Zener polaron phase (ZP) proposed in 2002 by Daoud-Aladine et al. [Phys. Rev. Lett. 89, 097205]), though formed by a pair of parallel Mn spins of different…
We perform spin wave analysis of classical ground states of a model Hamiltonian proposed earlier(Phys. Rev. B {\bf 90}, 104420(2014)) for $α-MnO_2$ compounds. It is known that the phase diagram of the Hollandite lattice (lattice of $α-MnO_2$ compounds) consists of four different Helical phases(FH, A2H, C2H, CH phase) in the space of model parameters $J_1,~J_2,~J_3$. The spin wave dispersion shows presence of gapless mode which interpolates between quadratic to linear depending on phases and values of $J_i$'s. In most cases, the 2nd lowest mode shows the existence of a roton minima mainly from …
Neutron scattering results are presented for spin-wave excitations of three ferromagnetic metallic $A_{1-x}A^{\prime}_{x}$MnO$_3$ manganites (where $A$ and $A^\prime$ are rare- and alkaline-earth ions), which when combined with previous work elucidate systematics of the interactions as a function of carrier concentration $x$, on-site disorder, and strength of the lattice distortion. The long wavelength spin dynamics show only a very weak dependence across the series. The ratio of fourth to first neighbor exchange ($J_4/J_1$) that controls the zone boundary magnon softening changes systematical…
Non-collinear two-dimensional triangular lattice antiferromagnets (2D TLAF) are currently an area of very active research due to their unique magnetic properties, which lead to non-trivial quantum effects that experimentally manifest themselves in the spin excitation spectra. Recent examples of such insulating 2D TLAF include (Y,Lu)MnO$_3$, LiCrO$_2$, and CuCrO$_2$. Hexagonal LuFeO3 is a recently synthesized 2D TLAF which exhibits properties of an ideal multiferroic material, partially because of the high spin ($S=5/2$) and strong magnetic super-exchange interactions. We report the full range …
