Neutron scattering study of ferroelectric Sn2P2S6 under pressure

Ferroelectric phase transition in the semiconductor Sn2P2S6 single crystal has been studied by means of neutron scattering in the pressure-temperature range adjacent to the anticipated tricritical Lifshitz point (p=0.18GPa, T=296K). The observations reveal a direct ferroelectric-paraelectric phase transition in the whole investigated pressure range (0.18 - 0.6GPa). These results are in a clear disagreement with phase diagrams assumed in numerous earlier works, according to which a hypothetical intermediate incommensurate phase extends over several or even tens of degrees in the 0.5GPa pressure range. Temperature dependence of the anisotropic quasielastic diffuse scattering suggests that polarization fluctuations present above TC are strongly reduced in the ordered phase. Still, the temperature dependence of the (200) Bragg reflection intensity at p=0.18GPa can be remarkably well modeled assuming the order-parameter amplitude growth according to the power law with logarithmic corrections predicted for a uniaxial ferroelectric transition at the tricritical Lifshitz point

Terahertz and infrared spectroscopic evidence of phonon-paramagnon coupling in hexagonal piezomagnetic YMnO3

Terahertz and far-infrared electric and magnetic responses of hexagonal piezomagnetic YMnO3 single crystals are investigated. Antiferromagnetic resonance is observed in the spectra of magnetic permeability mu_a [H(omega) oriented within the hexagonal plane] below the Neel temperature T_N. This excitation softens from 41 to 32 cm-1 on heating and finally disappears above T_N. An additional weak and heavily-damped excitation is seen in the spectra of complex dielectric permittivity epsilon_c within the same frequency range. This excitation contributes to the dielectric spectra in both antiferromagnetic and paramagnetic phases. Its oscillator strength significantly increases on heating towards room temperature thus providing evidence of piezomagnetic or higher-order couplings to polar phonons. Other heavily-damped dielectric excitations are detected near 100 cm-1 in the paramagnetic phase in both epsilon_c and epsilon_a spectra and they exhibit similar temperature behavior. These excitations appearing in the frequency range of magnon branches well below polar phonons could remind electromagnons; however, their temperature dependence is quite different. We have used density functional theory for calculating phonon dispersion branches in the whole Brillouin zone. A detailed analysis of these results and of previously published magnon dispersion branches brought us to the conclusion that the observed absorption bands stem from phonon-phonon and phonon- paramagnon differential absorption processes. The latter is enabled by a strong short-range in-plane spin correlations in the paramagnetic phase.Comment: subm. to PR

Magnetodielectric coupling and phonon properties of compressively strained EuTiO3 thin films deposited on LSAT

Compressively strained epitaxial (001) EuTiO3 thin films of tetragonal symmetry have been deposited on (001) (LaAlO3)_0.29-(SrAl_{1/2}Ta_{1/2}O3)_0.71 (LSAT) substrates by reactive molecular-beam epitaxy. Enhancement of the Neel temperature by 1 K with 0.9% compressive strain was revealed. The polar phonons ofthe films have been investigated as a function of temperature and magnetic field by means of infrared reflectance spectroscopy. All three infrared active phonons show strongly stiffened frequencies compared to bulk EuTiO3 in accordance with first principles calculations. The phonon frequencies exhibit gradual softening on cooling leading to an increase in static permittivity. A new polar phonon with frequency near the TO1 soft mode was detected below 150 K. The new mode coupled with the TO1 mode was assigned as the optical phonon from the Brillouin zone edge, which is activated in infrared spectra due to an antiferrodistortive phase transition and due to simultaneous presence of polar and/or magnetic nanoclusters. In the antiferromagnetic phase we have observed a remarkable softening of the lowest-frequency polar phonon under an applied magnetic field, which qualitatively agrees with first principles calculations. This demonstrates the strong spin-phonon coupling in EuTiO3, which is responsible for the pronounced dependence of its static permittivity on magnetic field in the antiferromagnetic phase.Comment: Submitted to Phys. Rev.

The Buffer Gas Beam: An Intense, Cold, and Slow Source for Atoms and Molecules

Beams of atoms and molecules are stalwart tools for spectroscopy and studies of collisional processes. The supersonic expansion technique can create cold beams of many species of atoms and molecules. However, the resulting beam is typically moving at a speed of 300-600 m/s in the lab frame, and for a large class of species has insufficient flux (i.e. brightness) for important applications. In contrast, buffer gas beams can be a superior method in many cases, producing cold and relatively slow molecules in the lab frame with high brightness and great versatility. There are basic differences between supersonic and buffer gas cooled beams regarding particular technological advantages and constraints. At present, it is clear that not all of the possible variations on the buffer gas method have been studied. In this review, we will present a survey of the current state of the art in buffer gas beams, and explore some of the possible future directions that these new methods might take

Lattice instabilities in bulk EuTiO3\mathrm{EuTiO_{3}}

The phase purity and the lattice dynamics in bulk EuTiO3 were investigated both microscopically, using x-ray and neutron diffraction, 151Eu-Mössbauer spectroscopy, and 151Eu nuclear inelastic scattering, and macroscopically using calorimetry, resonant ultrasound spectroscopy, and magnetometry. Furthermore, our investigations were corroborated by abinitio theoretical studies. The perovskite symmetry, Pm3¯m, is unstable at the M- and R-points of the Brillouin zone. The lattice instabilities are lifted when the structure relaxes in one of the symmetries: I4/mcm, Imma, R3¯c with relative relaxation energy around −25meV. Intimate phase analysis confirmed phase purity of our ceramics. A prominent peak in the Eu specific density of phonon states at 11.5meV can be modeled in all candidate symmetries. A stiffening on heating around room temperature is indicative of a phase transition similar to the one observed in SrTiO3, however, although previous studies reported the structural phase transition to the tetragonal I4/mcm phase our detailed sample purity analysis and thorough structural studies using complementary techniques did not confirm a direct phase transition. Instead, in the same temperature range, Eu delocalization is observed which might explain the lattice dynamical instabilities

Structure and thermoelectric properties of EuTi(O,N)3 ± δ

After partial substitution of nitrogen for oxygen in EuTiO3, the crystal structure, thermoelectric properties, morphology, and electronic structure of the products were analyzed and compared with pristine EuTiO3. The space group of EuTi(O,N)3 ±  δ was orthorhombic Pnma due to the tilt and rotation of the anion octahedra, compared to cubic Pm3¯m of EuTiO3 (at room temperature). The thermoelectric properties of oxynitride polycrystalline bodies sintered in three different ways were investigated in the temperature range of 300 K < T < 950 K. The Seebeck coefficients (S) of the oxynitrides were lower compared with the oxide, and the electrical resistivities (ρ) were increased about one order of magnitude. The activation energies (E A) indicated a larger band gap of EuTi(O,N)3 ±  δ when compared to the pristine EuTiO3 (∼1.3 eV compared to 0.98 eV). A morphological characterization by transmission electron microscopy and scanning electron microscopy illustrated intrinsic nanopores within the individual particles and weak grain-interconnections indicating poor intergrain electron transport. Ab initio calculations of the electronic structures confirmed a larger band gap of the distorted crystal structure of the oxynitride and showed a decrease of the density of states at the Fermi level, explaining the reduction of the measured S