We present data on the magnetic and magneto-elastic coupling in the hexagonal multiferroic manganite LuMnO3 from inelastic neutron scattering, magnetization and thermal expansion measurements. We measured the magnon dispersion along the main symmetry directions and used this data to determine the principal exchange parameters from a spin-wave model. An analysis of the magnetic anisotropy in terms of the crystal field acting on the Mn is presented. We compare the results for LuMnO3 with data on other hexagonal RMnO3 compounds.
We performed inelastic neutron scattering measurements on single crystals of NdFe$_{3}$($^{11}$BO$_{3}$)$_{4}$ to explore the magnetic excitations, to establish the underlying Hamiltonian, and to reveal the detailed nature of hybridization between the 4$f$ and 3$d$ magnetism. The observed spectra exhibiting a couple of key features, i.e., anti-crossing of Nd- and Fe-excitations and anisotropy gap at the antiferromagnetic zone center, are explained by the magnetic model including spin interaction in the framework of weakly-coupled Fe$^{3+}$ chains, interaction between the Fe$^{3+}$ and Nd$^{3+}…
We studied magnetic excitations in a low-temperature ferroelectric phase of the multiferroic YMn2O5 using inelastic neutron scattering (INS). We identify low-energy magnon modes and establish a correspondence between the magnon peaks observed by INS and electromagnon peaks observed in optical absorption [1]. Furthermore, we explain the microscopic mechanism, which results in the lowest-energy electromagnon peak, by comparing the inelastic neutron spectral weight with the polarization in the commensurate ferroelectric phase.
We report inelastic neutron scattering measurements that provide a distinct dynamical "fingerprint" for the multiferroic ground state of 3.5% Ga-doped CuFeO_2. The complex ground state is stabilized by the displacement of the oxygen atoms, which are also responsible for the multiferroic coupling predicted by Arima. By comparing the observed and calculated spectrum of spin excitations, we conclude that the magnetic ground state is a distorted screw-type spin configuration that requires a mechanism for magnetoelectric coupling different from the generally accepted spin-current model.
We report single-crystal neutron diffraction study of the magnetic structure of the multiferroic compound YbMnO$_3$, a member of the hexagonal manganite family, in zero-field and under a magnetic field applied along the $c$-axis. We propose a scenario for the zero-field magnetic ordering and for the field-induced magnetic reorientation of the Mn and of the two Yb on distinct crystallographic sites, compatible with the macroscopic measurements, as well as with previous powder neutron diffraction experiment and results from other techniques (optical second harmonic generation, Mössbauer spectros…
Electric control of multiferroic domains is demonstrated through polarized magnetic neutron diffraction. Cooling to the cycloidal multiferroic phase of Ni3V2O8 in an electric field (E) causes the incommensurate Bragg reflections to become neutron spin polarizing, the sense of neutron polarization reversing with E. Quantitative analysis indicates the E-treated sample has handedness that can be reversed by E. We further show close association between cycloidal and ferroelectric domains through E-driven spin and electric polarization hysteresis. We suggest that definite cycloidal handedness is ac…
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…
Interplay of Spin Waves, Crystal-Field Excitations, and Phonons in Multiferroic Ba3HoRu2O9 revealed by Inelastic Neutron Scattering, Crystal-Field Analysis, and Machine-Learned Phonon Calculations
Rajiv Gandhi Institute of Petroleum Technology（Rajiv Gandhi石油技术学院）；ISIS Neutron and Muon Source, STFC, Rutherford Appleton Laboratory（ISIS中子与缪子源，STFC，卢瑟福阿普顿实验室）；School of Physical Sciences, Indian Institute of Technology Goa（印度理工学院果阿分校物理科学学院）；UGC - DAE Consortium for Scientific Research Mumbai Centre, Bhabha Atomic Research Centre（UGC-DAE科学研究中心孟买中心，巴哈原子研究中心）；Highly Correlated Matter Research Group, Physics Department, University of Johannesburg（约翰内斯堡大学高度关联物质研究组物理系）
We report a comprehensive inelastic neutron scattering study of the hybrid molecule-based multiferroic compound (ND4)2FeCl5D2O in the zero-field incommensurate cycloidal phase and the high-field quasi-collinear phase. The spontaneous electric polarization changes its direction concurrently with the field-induced magnetic transition, from mostly aligned with the crystallographic a-axis to the c-axis. To account for such change of polarization direction, the underlying multiferroic mechanism was proposed to switch from the spin-current model induced via the inverse Dzyalloshinskii-Moriya interac…
We report on spherical neutron polarimetry and unpolarized neutron diffraction in zero magnetic field as well as flipping ratio and static magnetization measurements in high magnetic fields on the multiferroic square lattice antiferromagnet Ba$_2$CoGe$_2$O$_7$. We found that in zero magnetic field the magnetic space group is $Cm'm2'$ with sublattice magnetization parallel to the [100] axis of this orthorhombic setting. The spin canting has been found to be smaller than $0.2^\circ$ in the ground state. This assignment is in agreement with the field-induced changes of the magnetic domain structu…
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…
We report a comprehensive specific heat and inelastic neutron scattering study to explore the possible origin of multiferroicity in HoCrO$_3$. We have performed specific heat measurements in the temperature range 100 mK - 290 K and inelastic neutron scattering measurements were performed in the temperature range 1.5 - 200 K. From the specific heat data we determined hyperfine splitting at 22.5(2) $μ$eV and crystal field transitions at 1.379(5) meV, 10.37(4) meV, 15.49(9) meV and 23.44(9) meV, indicating the existence of strong hyperfine and crystal field interactions in HoCrO$_3$. Further, an …
Neutron diffraction and nuclear quadrupole resonance (NQR) measurements were employed to investigate magnetic order in the non-ferroelectric phase preceding the low-temperature multiferroic state in FeTe2O5Br. Refnement of the neutron diffraction data and simulations of 79,81Br NQR spectra reveal that the incommensurate magnetic ordering in the non-ferroelectric state comprises amplitude-modulated magnetic moments, similarly as in the multiferroic state. The two ordered states differ in the orientation of the magnetic moments and phase shifts between modulation waves. Surprisingly, all symmetr…
We have performed polarized and unpolarized small angle neutron scattering experiments on single crystals of HoMnO3 and have found that an increase in magnetic scattering at low momentum transfers begins upon cooling through temperatures close to the spin reorientation transition at TSR ~ 40 K. We attribute the increase to an uncompensated magnetization arising within antiferromagnetic domain walls. Polarized neutron scattering experiments performed while applying an electric field show that the field suppresses magnetic scattering below T ~ 50 K, indicating that the electric field affects the…
The magnetic properties of RMn2O5 multiferrroics as obtained by unpolarized and polarized neutron diffraction experiments are reviewed. We discuss the qualitative features of the magnetic phase diagram both in zero magnetic field and in field and analyze the commensurate magnetic structure and its coupling to an applied electric field. The origin of ferrolectricity is discussed based on calculations of the ferroelectric polarization predicted by different microscopic coupling mechanisms (exchange striction and cycloidal spin-orbit models). A minimal model containing a small set of parameters i…
By using polarized inelastic neutron scattering measurements, we show that the spin-lattice quantum entanglement in mutliferroics results in hybrid elementary excitations, involving spin and lattice degrees of freedom. These excitations can be considered as multiferroic Godstone modes. We argue that the Dzyaloshinskii-Moriya interaction could be at the origin of this hybridization.
For a symmetry consistent theoretical description of the multiferroic phase of Ba$_2$CoGe$_2$O$_7$ a precise knowledge of its crystal structure is a prerequisite. In our previous synchrotron X-ray diffraction experiment on multiferroic Ba$_2$CoGe$_2$O$_7$ at room temperature we found forbidden reflections that favour the tetragonal-to-orthorhombic symmetry lowering of the titled compound. Here, we report the results of room-temperature single-crystal diffraction studies with both hot and cold neutrons to differentiate between the real symmetry lowering and multiple diffraction (the Renninger e…
We report the magnetic diffraction pattern and spin wave excitations in (CD$_3$)$_2$ND$_2$[Mn(DCO$_2$)$_3$] measured using elastic and inelastic neutron scattering. The magnetic structure is shown to be a G-type antiferromagnet with moments pointing along the $b$ axis. By comparison with simulations based on linear spin wave theory, we have developed a model for the magnetic interactions in this multiferroic metal-organic framework material. The interactions form a three-dimensional network with antiferromagnetic nearest-neighbour interactions along three directions of $J_1=-0.103(8)$~meV, $J_…
We have studied the high temperature multiferroic cupric oxide using polarized neutron diffraction as a function of temperature and applied electric field. We find that the chiral domain population can be varied using an external electric field applied along the b axis. Using representation analysis we derive the incommensurate magnetic structure in the multiferroic phase. The origin of the magnetoelectric coupling is consistent with models based on the inverse Dzyaloshinskii-Moriya interaction, but is different from the simple cycloidal mechanism.
Magnetic order of the manganese and rare-earth lattices according to different symmetry representations is observed in multiferroic hexagonal (h-) DyMnO$_3$ by optical second harmonic generation and neutron diffraction. The incompatibility reveals that the 3d-4f coupling in the h-$R$MnO$_3$ system ($R$ = Sc, Y, In, Dy - Lu) is substantially less developed than commonly expected. As a consequence, magnetoelectric coupling effects in this type of split-order parameter multiferroic that were previously assigned to a pronounced 3d-4f coupling have now to be scrutinized with respect to their origin…
Anisotropic multiferroic properties of SrMnGe2O6 pyroxene single crystals were systematically investigated by means of magnetization, heat capacity, pyroelectric current measurement and elastic and inelastic neutron scattering experiments. Single crystal neutron diffraction allows us to unambiguously reveal the presence of two incommensurate magnetic orderings: a non-polar amplitude-modulated collinear sinusoidal magnetic structure emerges at TN1=4.36(2)K followed by a polar elliptical cycloidal spin structure below TN2=4.05(2)K. Pyroelectric current measurements on single crystal confirm the …
The layered compound KCu$_3$As$_2$O$_7$(OD)$_3$, comprising distorted kagome planes of $S=1/2$ Cu$^{2+}$ ions, is a recent addition to the family of type-II multiferroics. Previous zero field neutron diffraction work has found two helically ordered regimes in \kns, each showing a distinct coupling between the magnetic and ferroelectric order parameters. Here, we extend this work to magnetic fields up to $20$~T using neutron powder diffraction, capacitance, polarization, and high-field magnetization measurements, hence determining the $H-T$ phase diagram. We find metamagnetic transitions in bot…
By combining bulk properties, neutron diffraction and non-resonant X-ray diffraction measurements, we demonstrate that the new multiferroic Cu$_3$Nb$_2$O$_8$ becomes polar simultaneously with the appearance of generalised helicoidal magnetic ordering. The electrical polarization is oriented perpendicularly to the common plane of rotation of the spins --- an observation that cannot be reconciled with the "conventional" theory developed for cycloidal multiferroics. Our results are consistent with coupling between a macroscopic structural rotation, which is allowed in the paramagnetic group, and …
The chiral components in the magnetic order in multiferroic MnWO4 have been studied by neutron diffraction using spherical polarization analysis as a function of temperature and of external electric field. We show that sufficiently close to the ferroelectric transition it is possible to switch the chiral component by applying moderate electric fields at constant temperature. Full hysteresis cycles can be observed which indicate strong pinning of the magnetic order. MnWO4, furthermore, exhibits a magnetoelectric memory effect across heating into the paramagnetic and paraelectric phase.
High resolution inelastic neutron scattering reveals that the elementary magnetic excitations in multiferroic MnWO4 consist of low energy dispersive electromagnons in addition to the well-known spin-wave excitations. The latter can well be modeled by a Heisenberg Hamiltonian with magnetic exchange coupling extending to the 12th nearest neighbor. They exhibit a spin-wave gap of 0.61(1) meV. Two electromagnon branches appear at lower energies of 0.07(1) meV and 0.45(1) meV at the zone center. They reflect the dynamic magnetoelectric coupling and persist in both, the collinear magnetic and parael…
Magnetic structure of the multiferroic Ca$_{2}$CoSi$_{2}$O$_{7}$ was determined by neutron diffraction techniques. Combination of the polycrystalline and single-crystal samples experiments revealed a collinear antiferromagnetic structure with the easy axis along $<$100$>$ directions. The dielectric state was discussed in the framework of the spin-dependent $d$-$p$ hybridization mechanism, leading to the realization of the antiferroelectric structure. The origin of the magnetic anisotropy was discussed in comparison with the isostructural Ba$_{2}$CoGe$_{2}$O$_{7}$.
The field-induced multiferroic transition in TbMnO3 has been studied by neutron scattering. Apart strong hysteresis, the magnetic transition associated with the flop of electronic polarization exhibits a memory effect: after a field sweep, TbMnO3 does not exhibit the same phase as that obtained by zero-field cooling. The strong changes in the magnetic excitations across the transition perfectly agree with a rotation of the cycloidal spiral plane indicating that the inverse Dzyaloshinski-Moriya coupling causes the giant magnetoelectric effect at the field-induced transition. The analysis of the…
Neutron powder diffraction and single crystal x-ray resonant magnetic scattering measurements suggest that Dy plays an active role in enhancing the ferroelectric polarization in multiferroic DyMnO3 above TNDy = 6.5 K. We observe the evolution of an incommensurate ordering of Dy moments with the same periodicity as the Mn spiral ordering. It closely tracks the evolution of the ferroelectric polarization which reaches a maximum value of 0.2 muC/m^2. Below TNDy, where Dy spins order commensurately, the polarization decreases to values similar for those of TbMnO3.
The inelastic neutron scattering spectrum in cuprate superconductors is discussed on the basis of the itinerant-localized duality model for strongly correlated electrons. In Appendix the consistency with recent rigorous theoretical result on ARPES is discussed.
We present single-crystal neutron diffraction measurements on multiferroic LuFe2O4 showing phase transitions at 240 and 175 K. Magnetic reflections are observed below each transition indicating that the magnetic interactions in LuFe2O4 are 3-dimensional (3D) in character. The magnetic structure is refined as a ferrimagnetic spin configuration below the 240 K transition. While 3D magnetic correlations persists below 175 K, a significant broadening of the magnetic peaks is observed along with the build up of a diffuse component to the magnetic scattering.
We have investigated the crystal and magnetic structures of the trigonal iron-boracite Fe3B7O13X with X = OH by neutron diffraction. Neutron diffraction enables us to locate the hydrogen atom of the hydroxyl group and determine the magnetic ground state of this member of the multiferroic boracite family. No evidence was found for a monoclinic distortion in the magnetic ordered state. The magnetic symmetry allows for magnetoelectric and ferroelectric properties. The N/'eel tempera- ture TN of 4.86(4) K confirms the general trends within the boracites that TN decreases from X = I > Br > Cl > OH.…
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…
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 …
We demonstrate the existence of the spin nematic interactions in an easy-plane type antiferromagnet Ba$_{2}$CoGe$_{2}$O$_{7}$ by exploring the magnetic anisotropy and spin dynamics. Combination of neutron scattering and magnetic susceptibility measurements reveals that the origin of the in-plane anisotropy is an antiferro-type interaction of the spin nematic operator. The relation between the nematic operator and the electric polarization in the ligand symmetry of this compound is presented. The introduction of the spin nematic interaction is useful to understand the physics of spin and electr…
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…
Single-crystal samples of LiCu2O2 with spin 1/2 Cu2+ chains of edge-sharing CuO4 square planes (ribbon chains), have been characterized by X-ray diffraction, thermogravimetric analysis, and magnetic measurements. Neither the atomic deficiency nor the mixing of Cu and Li atoms has been found, indicating that lattice defects conceived as a possible origin of the reported multiferroic behavior can be excluded. Anomalies found in the data of specific heat and neutron magnetic Bragg reflections show clear evidence that the system exhibits successive magnetic transitions at TN1=24.5 K and TN2=22.8 K…
We have carried out neutron diffraction and small angle neutron scattering measurements on a high quality single crystal of the cubic lacunar spinel multiferroic, GaV$_4$S$_8$, as a function of magnetic field and temperature to determine the magnetic properties for the single electron that is located on the tetrahedrally coordinated V$_4$ molecular unit. Our results are in good agreement with the structural transition at 44 K from cubic to rhombohedral symmetry where the system becomes a robust ferroelectric, while long range magnetic order develops below 13 K in the form of an incommensurate …
We have combined neutron scattering and piezoresponse force microscopy to study the relation between the exchange bias observed in CoFeB/BiFeO3 heterostructures and the multiferroic domain structure of the BiFeO3 films. We show that the exchange field scales with the inverse of the ferroelectric and antiferromagnetic domain size, as expected from Malozemoff's model of exchange bias extended to multiferroics. Accordingly, polarized neutron reflectometry reveals the presence of uncompensated spins in the BiFeO3 film at the interface with the CoFeB. In view of these results we discuss possible st…
The coupling of magnetic chiralities to the ferroelectric polarisation in multiferroic RbFe(MoO$_4$)$_2$ is investigated by neutron spherical polarimetry. Because of the axiality of the crystal structure below $T_\textrm{c}$ = 190 K, helicity and triangular chirality are symmetric-exchange coupled, explaining the onset of the ferroelectricity in this proper-screw magnetic structure - a mechanism that can be generalised to other systems with "ferroaxial" distortions in the crystal structure. With an applied electric field we demonstrate control of the chiralities in both structural domains simu…
Using polarized inelastic neutron scattering the antisymmetric part of the dynamical susceptibility in non-centrosymmetric MnSi is determined. The paramagnetic fluctuations are found to be incommensurate with the chemical lattice and to have a chiral character. We show that antisymmetric interactions must be taken into account to properly describe the critical dynamics in MnSi above the Curie temperature. The inelastic neutron data is interpreted within the framework of the SCR-theory, taking into account the Dzyaloshinskii-Moriya interaction.
We report a single crystal neutron and x-ray diffraction study of the hybrid improper multiferroic Ca3Mn1.9Ti0.1O7 (CMTO), a prototypical system where the electric polarization arises from the condensation of two lattice distortion modes.With increasing temperature (T ), the out-of-plane, antiphase tilt of MnO6 decreases in amplitude while the in-plane, in-phase rotation remains robust and experiences abrupt changes across the first-order structural transition. Application of hydrostatic pressure (P) to CMTO at room temperature shows a similar effect. The consistent behavior under both T and P…
We performed magnetic and ferroelectric measurements, associated with Landau theory and symmetry analysis, in order to clarify the situation of the YMnO3 system, a classical example of type I multiferroics. We found that the only magnetic group compatible with all experimental data (neutrons scattering, magnetization,polarization, dielectric constant, second harmonic generation) is the P6'3 group. In this group a small ferromagnetic component along c is induced by the Dzyaloshinskii-Moriya interaction, and observed here in SQUID magnetization measurements. We found that the ferromagnetic and a…
Using in-field single crystal neutron diffraction we have determined the magnetic structure of TbMnO3 in the high field P||a phase. We unambiguously establish that the ferroelectric polarization arises from a cycloidal Mn spins ordering, with spins rotating in the ab plane. Our results demonstrate directly that the flop of the ferroelectric polarization in TbMnO3 with applied magnetic field is caused from the flop of the Mn cycloidal plane.
We have demonstrated that ferroelectric polarization in a spin-driven multiferroic CuFe1-xGaxO2 with x = 0.035 can be controlled by the application of uniaxial pressure. Our neutron diffraction and in-situ ferroelectric polarization measurements have revealed that the pressure dependence of the ferroelectric polarization is explained by repopulation of three types of magnetic domains originating from the trigonal symmetry of the crystal. We conclude that the spin-driven anisotropic lattice distortion and the fixed relationship between the directions of the magnetic modulation wave vector and t…
We have performed high resolution neutron diffraction and inelastic neutron scattering experiments in the frustrated multiferroic hexagonal compounds RMnO3 (R=Ho, Yb, Sc, Y), which provide evidence of a strong magneto-elastic coupling in the the whole family. We can correlate the atomic positions, the type of magnetic structure and the nature of the spin waves whatever the R ion and temperature. The key parameter is the position of the Mn ions in the unit cell with respect to a critical threshold of 1/3, which determines the sign of the coupling between Mn triangular planes.
Non-resonant X-ray magnetic scattering has been used to study the magnetic structure of multiferroic TbMnO3 in its ferroelectric phase. Circularly polarized X-rays were combined with a full polarization analysis of the scattered beam to reveal important new information on the magnetic structure of this canonical multiferroic. An applied electric field is shown to create a magnetic nearly mono-domain state in which the cylcoidal order on the Mn sublattice rotates either clockwise or counter-clockwise depending on the sign of the field. It is demonstrated how this technique provides sensitivity …
The magnetic form factor of YbInNi4 has been determined via the flipping ratios R with polarized neutron diffraction and the scattering function S(Q,w) was measured in an inelastic neutron scattering experiment. Both experiments were performed with the aim to determine the crystal-field scheme. The magnetic form factor clearly excludes the possibility of a \Gamma7 doublet as the ground state. The inelastic neutron data exhibit two, almost equally strong peaks at 3.2 meV and 4.4 meV which points, in agreement with earlier neutron data, towards a \Gamma8 quartet ground state. Further possibiliti…
In this short note, we report on the first inelastic neutron scattering (INS) study on high-energy magnetic excitations in Sr$_3$Ir$_2$O$_7$. We observed excitations between $\sim$80 meV and $\sim$180 meV. The peak position of the excitations is consistent with the dispersion of a single magnon determined by resonant inelastic X-ray scattering (RIXS) measurement. Thus, our results demonstrate that INS and RIXS observe identical excitations in iridate oxides, as in La$_2$CuO$_4$.
We have performed synchrotron radiation X-ray and neutron diffraction measurements on magnetoelectric multiferroic CuFe1-xAlxO2 (x=0.0155), which has a proper helical magnetic structure with incommensurate propagation wave vector in the ferroelectric phase. The present measurements revealed that the ferroelectric phase is accompanied by lattice modulation with a wave number 2q, where q is the magnetic modulation wave number. We have calculated the Fourier spectrum of the spatial modulations in the local electric polarization using a microscopic model proposed by Arima [T. Arima, J. Phys. Soc. …
We used Raman and terahertz spectroscopies to investigate lattice and magnetic excitations and their cross-coupling in the hexagonal YMnO3 multiferroic. Two phonon modes are strongly affected by the magnetic order. Magnon excitations have been identified thanks to comparison with neutron measurements and spin wave calculations but no electromagnon has been observed. In addition, we evidenced two additional Raman active peaks. We have compared this observation with the anti-crossing between magnon and acoustic phonon branches measured by neutron. These optical measurements underly the unusual s…
The high-energy phonons in La1.5Sr0.5NiO4, in which the checkerboard charge ordering is formed, was investigated by the inelastic neutron scattering. We found that the longitudinal modes show strong anomalies compared with La2NiO4. We argue the similarity and difference in the phonon anomalies between the present sample and the preceding works of different compositions.
The magnetic field induced rearrangement of the cycloidal spin structure in ferroelectric mono-domain single crystals of the room-temperature multiferroic BiFeO$_3$ is studied using small-angle neutron scattering (SANS). The cycloid propagation vectors are observed to rotate when magnetic fields applied perpendicular to the rhombohedral (polar) axis exceed a pinning threshold value of $\sim$5\,T. In light of these experimental results, a phenomenological model is proposed that captures the rearrangement of the cycloidal domains, and we revisit the microscopic origin of the magnetoelectric effe…
Both the Dzyaloshiskii-Moriya interaction and the exchange-striction are shown to affect dynamically the magnetoelectric excitations in the perovskite multiferroic RMnO3. The exchange-striction results in a biquadratic interaction between the spins and the transverse phonons, giving rise to quantum fluctuations of the ferroelectric polarization P. This leads to low-lying phonon modes that are perpendicular to P and to the helical spins at small wave vector but are parallel to P at a wave vector close to the magnetic modulation vector. For spin-1/2 helimagnet, the local polarization can be comp…
The pressure ($p$) -- temperature ($T$) phase diagram for microscopic magnetism in the multiferroic compound HoMn$_{2}$O$_{5}$ was established using neutron diffraction measurements under a hydrostatic pressure up to 1.25 GPa. At ambient pressure, incommensurate--commensurate--incommensurate magnetic phase transitions occur successively with decreasing temperature. Upon applying pressure, the incommensurate phase at the lowest temperature almost decreases and the commensurate phase appears. The $p$ -- $T$ phase diagram established shows excellent agreement with the recently reported $p$ -- $T$…
A procedure is outlined for the determination of magnetic exchange constants in anisotropic perovskite anitferromagnets using powder inelastic neutron scattering. Spin wave densities-of-states are measured using time-of-flight inelastic neutron scattering for LaMnO$_{3}$ ($A$-type antiferromagnet), LaVO$_{3}$ ($C$-type), and LaFeO$_{3}$ ($G$-type) and compared to Heisenberg model calculations. The anisotropy of in-plane ($J_{ab}$) and out-of-plane ($J_{c}$) exchange constants can be obtained from the data. The procedure quickly determines the magnetic exchange interactions without the need for…
We present a 57Fe Mössbauer spectroscopy study of the two incommensurate magnetic phases in the multiferroic material FeVO4. We devise lineshapes appropriate for planar elliptical and collinear modulated magnetic structures and show that they reproduce very well the Mössbauer spectra in FeVO4, in full qualitative agreement with a previous neutron diffraction study. Quantitatively, our spectra provide precise determinations of the characteristics of the elliptical and modulated structures which are in good agreement with the neutron diffraction results. We find that the hyperfine field elliptic…
High-energy, local multiplet excitations of the d-electrons are revealed in our inelastic neutron scattering measurements on the prototype magnetic insulator NiO. These become allowed by the presence of both non-zero crystal field and spin-orbit coupling. The observed excitations are consistent with optical, x-ray, and EELS measurements of d-d excitations. This experiment serves as a proof of principle that high-energy neutron spectroscopy is a reliable and useful technique for probing electronic excitations in systems with significant crystal field and spin-orbit interactions.
Inelastic neutron scattering (INS) is one powerful technique to study the low-energy single-spin dynamics of magnetic materials. A variety of quantum magnets show novel magnetic correlations such as quantum spin liquids. These novel magnetic correlations are beyond the direct detection of INS. In this paper we propose a coincidence technique, coincidence inelastic neutron scattering (cINS), which can detect the two-spin magnetic correlations of the magnetic materials. In cINS there are two neutron sources and two neutron detectors with an additional coincidence detector. Two neutrons from the …
