Temperature‐dependent Raman scattering study of multiferroic MnWO4

We have measured polarized Raman spectra of MnWO₄ single crystals at low temperatures, and studied the temperature dependence of the various phonon modes. From our Raman studies of the MnWO₄, a new transition temperature, ∼180 K, was found. We have completely assigned the symmetries of the 18 observed Raman modes of the MnWO₄, as expected from a group theoretical analysis. These Raman modes have been classified into three groups according to weak, intermediate and strong temperature dependence of the modes in each group. Six internal modes have been identified by their weak temperature dependence of the Raman wavenumbers. The temperature dependence of the wavenumbers of the B_g modes in Mg O bonds, modes of intermediate temperature dependence group, shows an anomalous behavior under 50 K. The phonon modes of strong temperature dependence show an anomalous change at ∼180 K in the linewidths. This is believed to be a new transition temperature which involves the changes in the inter‐WO₆ octahedra structure. Copyright © 2009 John Wiley & Sons, Ltd.     

Spin-wave excitations in superlattices self-assembled in multiferroic single crystals

Spin-wave excitations revealed in the dynamically equilibrated one-dimensional superlattices formed due to phase separation and charge carrier self-organization in doped single crystals of Eu(0.8)Ce(0.2)Mn(2)O(5) and Tb(0.95)Bi(0.05)MnO(3) multiferroics are discussed. Similar excitations, but having lower intensities, were also observed in undoped RMn(2)O(5) (R=Eu, Er, Tb, Bi). This suggests that a charge transfer between manganese ions with different valences, which give rise to the superlattice formation, occurs in undoped multiferroics as well. The spin excitations observed in the native superlattices represent a set of homogeneous spin-wave resonances excited in individual superlattice layers. The positions of these resonances depend on the relation between the numbers of Mn(3+) and Mn(4+) ions, charge carrier concentrations, and barrier depths in the superlattice layers. It has been found that the spin-wave excitations observed in the frequency interval studied (30-50?GHz) form two spin-wave minibands with a gap between them.     

Low energy excitations in CeNiSn

We have studied the magnetic excitation spectrum of CeNiSn at low energies both on a polycrystalline sample using time-of-flight technique and on a single crystal with a triple axis spectrometer. The energy gap in the excitation spectrum is clearly observed in the polycrystalline sample reconciling the earlier discrepancies between the two kinds of measurements. The experimental results are consistent with the occurrence of a quasielastic signal within the gap without any significant wave vector dependence and characterized by an energy scale Γ≈0.2 meV.     

Low energy excitations in amorphous metals

The low temperature properties of amorphous metals pertinent to the existence of low energy excitations are reviewed. In an introductory section, the currently accepted model for low energy excitations, i.e. the model of two level systems (TLS), is discussed. The treatment of amorphous metals focuses on the specific heat C, thermal conductivity κ, ultrasonic properties and electrical resistivity ?. Measurements of C and κ are often performed on amorphous superconductors in order to exclude the effect of conduction electrons. The TLS density of states and the TLS-phonon coupling in these materials as determined from C and κ respectively are surprisingly close to values for insulating glasses. Ultrasonic experiments carried out mostly on normal amorphous metals reveal a strongly enhanced TLS relaxation rate with respect to insulators. This can be attributed to TLS-electron coupling. The effect of this coupling on ? is uncertain at present. In order to obtain more insight into the microscopic origin of TLS in metallic and insulating glasses some examples of TLS in crystalline disordered solids are discussed. Finally, some formal analogies are drawn between spin glasses and real glasses.     

Low energy excitations in spin glasses

We discuss the nature of excitations that govern the low temperature thermodynamic behaviour of spin glasses and propose that the spin glass state is a space-time dependent ground state of a system of interacting spins wherein rotational invariance is broken spontaneously.     

Charge-transfer excitations in the model superconductor HgBa(2)CuO(4+delta)

We report a Cu -edge resonant inelastic x-ray scattering (RIXS) study of charge-transfer excitations in the 2-8 eV range in the structurally simple compound HgBa(2)CuO(4+delta) at optimal doping (T(c)=96.5 K). The spectra exhibit a significant dependence on the incident photon energy which we carefully utilize to resolve a multiplet of weakly dispersive (<0.5 eV) electron-hole excitations, including a mode at 2 eV. The observation of this 2 eV excitation suggests the existence of a remnant charge-transfer gap deep in the superconducting phase. Quite generally, our results, which include additional data for the Mott insulator La(2)CuO(4), demonstrate the importance of exploring the incident photon-energy dependence of the RIXS cross section.     

Magnetic excitations in multiferroic TbMnO3: evidence for a hybridized soft mode

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 2.5 meV correspond to rotations of the spiral rotation plane. These latter modes are expected to couple to the electric polarization. The 2.5 meV mode is in perfect agreement with recent infrared-spectroscopy data giving strong support to its interpretation as a hybridized phonon-magnon excitation.     

Crystal field and exchange interactions in the SmFe3(BO3)4 multiferroic

The optical spectra of oriented SmFe₃(BO₃)₄ single crystals are studied in the region of the f-f transitions in the Sm³⁺ ion by Fourier spectroscopy. The energies, the symmetry properties, and the exchange splittings of the Stark sublevels of the ground and 17 excited multiplets of the Sm³⁺ ion in a crystal field of symmetry D ₃ are determined from the measured temperature dependences of polarized-radiation absorption spectra. The parameters of the crystal field acting on samarium ions and the parameters of the exchange interaction between Sm³⁺ and Fe³⁺ ions are found. The anisotropy of the effective exchange interaction is shown to be substantially stronger than the magnetic anisotropy, due to a strong crystal-field-induced mixing of the ground and excited multiplets.     

Far-infrared optical excitations in multiferroic TbMnO<Subscript>3</Subscript>

We provide a detailed study of the reflectivity of multiferroic TbMnO₃ for wave numbers from 40 cm^-1 to 1000 cm^-1 and temperatures 5 K < T < 300 K. Excitations are studied for polarization directions E || a, the polarization where electromagnons are observed, and for E || c, the direction of the spontaneous polarization in this material. The temperature dependencies of eigenfrequencies, damping constants and polar strengths of all modes are studied and analyzed. For E || a and below the spiral ordering temperature of about 27 K we observe a transfer of optical weight from phonon excitations to electromagnons, which mainly involves low-frequency phonons. For E || c an unusual increase of the total polar strength and hence of the dielectric constant is observed indicating significant transfer of dynamic charge probably within manganese-oxygen bonds on decreasing temperatures.     

Resonant inelastic x-ray scattering study of charge excitations in La(2)CuO(4)

We report a resonant inelastic x-ray scattering study of the dispersion relations of charge-transfer excitations in insulating La(2)CuO(4).. These data reveal two peaks, both of which show two-dimensional characteristics. The lowest energy excitation has a gap energy of approximately 2.2 eV at the zone enter, and a dispersion of approximately 1 eV. The spectral weight of this mode becomes dramatically smaller around (pi, pi). The second peak shows a smaller dispersion ( approximately 0.5 eV) with a zone-center energy of approximately 3.9 eV. We argue that these are both highly dispersive exciton modes damped by the presence of the electron-hole continuum.     

Evidence for an electric-dipole active continuum band of spin excitations in multiferroic TbMnO3

The wide range optical spectra on a multiferroic prototype TbMnO3 have been investigated to clarify the origin of spin excitations observed in the far-infrared region. We elucidate the full band structure, whose high energy edge (133 cm;{-1}) exactly corresponds to twice of the highest-lying magnon energy. Thus the origin of this absorption band is clearly assigned to two-magnon excitation driven by the electric field of light. There is an overlap between the two-magnon and phonon energy ranges, where the strong coupling between them is manifested by the frequency shift and transfer of oscillator strength of the phonon mode.     

Low lying excitations in a pair-potential well

Recently a new method has been developed for solving the Bogoliubov equations in the absence of magnetic field. In this work we apply the method to calculate low-Lying bound states in a paramagnetic-superconducting contact. It is assumed that the pairpotential drops from its bulk value inside the superconductor to zero at the interface, with finite slope. Impurity scattering is neglected. No sharp energy gap is found in the limit of vanishing thickness of the paramagnetic normal layer contrary to former work. The influence of neglecting a small term in the kinetic energy investigated. It is shown that for bound states the correction to the energy due to this term in the first order perturbation theory is zero.     

Large tunable FMR frequency shift by magnetoelectric coupling in oblique-sputtered Fe_(52.5)Co_(22.5)B_(25.0)/PZN-PT multiferroic heterostructure

In this study, we observe a strong inverse magnetoelectric coupling in Fe_(52.5)Co_(22.5)B_(25.0)/PZN-PT multiferroic heterostructure, which produces large electric field(E-field) tunability of microwave magnetic properties. With the increase of the E-field from 0 to 8 kV/cm, the magnetic anisotropy field Heffis dramatically enhanced from 169 to 600 Oe, which further leads to a significant enhancement of ferromagnetic resonance frequency from 4.57 to 8.73 GHz under zero bias magnetic field, and a simultaneous decrease of the damping constant α from 0.021 to 0.0186. These features demonstrate that this multiferroic composite is a promising candidate for fabricating E-field tunable microwave components.     

Low lying octupole excitations in 15N

The inelastic electron scattering form factors for the $\text{5.27}\text{MeV}\text{(}\text{5}\text{2}{}^{\mathrm{+}}\text{), 7.15}\text{MeV}\text{(}\text{5}\text{2}{}^{\mathrm{+}}\text{), 7.30}\text{MeV}\text{(}\text{3}\text{2}{}^{\mathrm{+}}\text{)}\text{and}\text{7.56}\text{MeV}\text{(}\text{7}\text{2}{}^{\mathrm{+}}\text{)}$ levels have been measured in the momentum transfer range between 0.6 and 1.1 fm^?1. The resulting B(E3) values are discussed in terms of weak coupling models and the spherical shell model of Zuker, Buck and McGrory.     

Low frequency double electron muon resonance (Demur) in fused quartz

Double electron muon resonance was studied with comparable amplitudes of the static and rf magnetic fields. The experiments were carried out in fused quartz and employed a resonant linearly-polarized rf field and a small static field. For small amplitudes of the rf field a three-line frequency spectrum was obtained consisting of a central line at the rf frequency and two weaker lines of equal amplitude symmetrically positioned about the central line. A symmetrical three line spectrum is predicted for muonium using the rotating wave approximation (RWA). For large rf fields the amplitudes of the three lines were not symmetric and depended on whether positrons were observed parallel or perpendicular to the beam. For very large rf fields the total amplitude of all the lines was less than for lower rf fields. These results do not agree with the theory using the RWA and no satisfactory theory currently exists.     

Raman phonons in multiferroic FeVO_4 crystals

Multiferroic materials are promising candidates for next-generation multi-functional devices, because of the coexistence of multi-orders and the coupling between the orders. FeVO4 has been confirmed to be a multiferroic compound,since it exhibits both ferroelectricity and antiferromagnetic ordering at low temperatures. In this paper, we have performed careful Raman scattering measurements on high-quality Fe VO4 single crystals. The compound has a very rich phonon structure due to its low crystal symmetry(P- 1) and at least 47 Raman-active phonon modes have been resolved in the low and hightemperature spectra. Most of the observed modes are well assigned with aid of first-principles calculations and symmetry analysis. The present study provides an experimental basis for exploring spin-lattice coupling and the mechanism of multiferroicity in FeVO4     

Rotational excitations of NH 4 + in (NH4) x K1−x I

We propose a gaussian model for the distribution of rotational tunneling lines which constitute the experimentally observed inelastic neutron scattering spectra in the range 0 to 0.6 meV from the mixed system (NH₄) _x K_1−x I. The intensity profiles generated by this model are in remarkable agreement with the experimentally observed ones.     

Dielectric properties of (NH4)2SO4 crystals in the range of electronic excitations

Spectra of the real and imaginary parts of the pseudo‐dielectric permittivity, 〈?₁〉(E) and 〈?₂〉(E), of ferroelectric ammonium sulfate crystals, (NH₄)₂SO₄, have been measured in the range of electronic excitations 4.0 to 9.5 eV by ellipsometry using synchrotron radiation. Temperature dependences of the corresponding susceptibilities, 〈χ₁〉(T) and 〈χ₂〉(T), obtained for the photon energy E = 8.5 eV, related to excitations of oxygen p‐electrons, reveal sharp peak‐like temperature changes near the Curie point T_C = 223 K. The large temperature‐dependent increase of the imaginary part of the susceptibility χ₂(T), together with a simultaneous decrease of the real part of the susceptibility χ₁(T), take place at the phase transition. These anomalies have been ascribed mainly to the SO₄ group of the crystal structure.     

High-pressure Raman scattering and an anharmonicity study of multiferroic wolframite-type Mn(0.97)Fe(0.03)WO(4)

A high-pressure Raman scattering study of wolframite-type Mn(0.97)Fe(0.03)WO(4) is presented up to 10.4?GPa. The phonon wavenumbers vary linearly with pressure. The mode Grüneisen parameters are larger for many bending and lattice modes when compared to the stretching modes due to the larger compressibility of Mn(Fe)O(6) octahedra when compared to WO(6) octahedra. Combining the pressure-dependent Raman data of this work with the temperature-dependent Raman data on this crystal previously reported by us has allowed estimation of the temperature-dependent pure lattice and intrinsic anharmonic contributions to the observed total Raman shifts as a function of temperature. It has been found that the observed unusual hardening of the 884, 698 and 674?cm(-1) stretching modes upon heating from 4 to about 150-200?K followed by the usual softening above 150-200?K is a result of a positive intrinsic anharmonic contribution and a negative pure lattice contribution; i.e.,?up to about 150-200?K the anharmonic contribution surpasses the lattice contribution and the total Raman shift is slightly positive whereas above 150-200?K the lattice contribution becomes dominant and the Raman bands exhibit the usual softening with increasing temperature.