46 research outputs found
Antiferrodistortive phase transition in EuTiO3
X-ray diffraction, dynamical mechanical analysis and infrared reflectivity
studies revealed an antiferrodistortive phase transition in EuTiO3 ceramics.
Near 300K the perovskite structure changes from cubic Pm-3m to tetragonal
I4/mcm due to antiphase tilting of oxygen octahedra along the c axis (a0a0c- in
Glazer notation). The phase transition is analogous to SrTiO3. However, some
ceramics as well as single crystals of EuTiO3 show different infrared
reflectivity spectra bringing evidence of a different crystal structure. In
such samples electron diffraction revealed an incommensurate tetragonal
structure with modulation wavevector q ~ 0.38 a*. Extra phonons in samples with
modulated structure are activated in the IR spectra due to folding of the
Brillouin zone. We propose that defects like Eu3+ and oxygen vacancies strongly
influence the temperature of the phase transition to antiferrodistortive phase
as well as the tendency to incommensurate modulation in EuTiO3.Comment: PRB, in pres
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.
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
Spin-phonon coupling in epitaxial Sr0.6Ba0.4MnO3 thin films
Spin-phonon coupling is investigated in epitaxially strained Sr1-xBaxMnO3 thin films with perovskite structure by means of microwave (MW) and infrared (IR) spectroscopy. In this work we focus on the Sr0.6Ba0.4MnO3 composition grown on (LaAlO3)0.3(Sr2AlTaO6)0.7 substrate. The MW complex electromagnetic response shows a decrease in the real part and a clear anomaly in the imaginary part around 150 K. Moreover, it coincides with a 17% hardening of the lowest-frequency polar phonon seen in IR reflectance spectra. In order to further elucidate this phenomenon, low-energy muon-spin spectroscopy was carried out, signaling the emergence of antiferromagnetic order with Néel temperature (TN) around 150 K. Thus, our results confirm that epitaxial Sr0.6Ba0.4MnO3 thin films display strong spin-phonon coupling below TN, which may stimulate further research on tuning the magnetoelectric coupling by controlling the epitaxial strain and chemical pressure in the Sr1-xBaxMnO3 system
First-principles design and subsequent synthesis of a material to search for the permanent electric dipole moment of the electron
We describe the first-principles design and subsequent synthesis of a new
material with the specific functionalities required for a solid-state-based
search for the permanent electric dipole moment of the electron. We show
computationally that perovskite-structure europium barium titanate should
exhibit the required large and pressure-dependent ferroelectric polarization,
local magnetic moments, and absence of magnetic ordering even at liquid helium
temperature. Subsequent synthesis and characterization of
EuBaTiO ceramics confirm the predicted desirable
properties.Comment: Nature Materials, in pres
Optical Response of DyN
We report measurements of the optical response of polycrystalline DyN thin
films. The frequency-dependent complex refractive index in the near
IR-visible-near UV was determined by fitting reflection/transmission spectra.
In conjunction with resistivity measurements these identify DyN as a
semiconductor with 1.2 eV optical gap. When doped by nitrogen vacancies it
shows free carrier absorption and a blue-shifted gap associated with the
Moss-Burstein effect. The refractive index of 2.0+/-0.1 depends only weakly on
energy. Far infrared reflectivity data show a polar phonon of frequency 280
cm-1 and dielectric strength delta epsilon= 20
Strong spin-phonon coupling in infrared and Raman spectra of SrMnO3
Infrared reflectivity spectra of cubic SrMnO3 ceramics reveal 18% stiffening of the lowest-frequency phonon below the antiferromagnetic phase transition occurring at T-N = 233 K. Such a large temperature change of the polar phonon frequency is extraordinary and we attribute it to an exceptionally strong spin-phonon coupling in this material. This is consistent with our prediction from first-principles calculations. Moreover, polar phonons become Raman active below T-N, although their activation is forbidden by symmetry in the Pm (3) over barm space group. This gives evidence that the cubic Pm (3) over barm symmetry is locally broken below T-N due to a strong magnetoelectric coupling. Multiphonon and multimagnon scattering is also observed in Raman spectra. Microwave and THz permittivity is strongly influenced by hopping electronic conductivity, which is caused by small nonstoichiometry of the sample. Thermoelectric measurements show room-temperature concentration of free carriers n(e) = 3.6 x 10(20) cm(-3) and the sample composition Sr2+Mn0.984+Mn0.023+O2.992-. The conductivity exhibits very unusual temperature behavior: THz conductivity increases on cooling, while the static conductivity markedly decreases on cooling. We attribute this to different conductivity of the ceramic grains and grain boundariesclose