Central mode and soft mode behavior in PbMg1/Nb2/3O3 relaxor ferroelectric

The relaxor ferroelectric PbMg1/Nb2/3O3 was investigated by means of broad-band dielectric and Fourier Transform Infrared (FTIR) transmission spectroscopy in the frequency range from 1 MHz to 15 THz at temperatures between 20 and 900 K using PMN films on infrared transparent sapphire substrates. While thin film relaxors display reduced dielectric permittivity at low frequencies, their high frequency intrinsic or lattice response is shown to be the same as single crystal/ceramic specemins. It was observed that in contrast to the results of inelastic neutron scattering, the optic soft mode was underdamped at all temperatures. On heating, the TO1 soft phonon followed the Cochran law with an extrapolated critical temperature equal to the Burns temperature of 670 K and softened down to 50 cm-1. Above 450 K the soft mode frequency leveled off and slightly increased above the Burns temperature. A central mode, describing the dynamics of polar nanoclusters appeared below the Burns temperature at frequencies near the optic soft mode and dramatically slowed down below 1 MHz on cooling below room temperature. It broadened on cooling, giving rise to frequency independent losses in microwave and lower frequency range below the freezing temperature of 200 K. In addition, a new heavily damped mode appeared in the FTIR spectra below the soft mode frequency at room temperature and below. The origin of this mode as well as the discrepancy between the soft mode damping in neutron and infrared spectra is discussed.Comment: 7 pages with 7 figures, submitted to Phys. Rev.

High-frequency dielectric spectroscopy of batio3 core - silica shell nanocomposites: Problem of interdiffusion

Three types of BaTiO3 core - amorphous nano-shell composite ceramics were processed from the same core-shell powder by standard sintering, spark-plasma sintering and two-step sintering techniques and characterized by XRD, HRSEM and broad-band dielectric spectroscopy in the frequency range 10^3 - 10^13 Hz including the THz and IR range. The samples differed by porosity and by the amount of interdiffusion from the cores to shells, in correlation with their increasing porosity. The dielectric spectra were also calculated using suitable models based on effective medium approximation. The measurements revealed a strong dielectric dispersion below the THz range, which cannot be explained by the modeling, and whose strength was in correlation with the degree of interdiffusion. We assigned it to an effect of the interdiffusion layers, giving rise to a strong interfacial polarization. It appears that the high-frequency dielectric spectroscopy is an extremely sensitive tool for detection of any gradient layers and sample inhomogeneities even in dielectric materials with negligible conductivity

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

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.

Fast polarization mechanisms in the uniaxial tungsten-bronze relaxor strontium barium niobate SBN-81

The high-frequency dielectric response of the uniaxial strontium barium niobate crystals with 81% of Sr has been studied from 1 kHz to 30 THz along the polar c axis by means of several techniques (far infrared, time domain terahertz, high-frequency and low-frequency dielectric spectroscopies) in a wide temperature interval 20–600 K. Relaxor properties were observed in the complex dielectric response and four main excitations were ascertained below the phonon frequencies. These fast polarization mechanisms take place at THz, GHz and MHz ranges and show different temperature evolution. The central mode excitation in the THz range, related to anharmonic dynamics of cations, slightly softens from high temperatures and then hardens below T ~ 400 K. Below the phase transition (at T ~ 330 K) an additional microwave excitation appears near 10 GHz related to micro domain wall oscillations. The strongest relaxation appears in the GHz range and slows down on cooling according to the Arrhenius law. Finally, another relaxation, present in the MHz range at high temperatures, also slows down on cooling at least to the kHz range. These two relaxations are due to polar fluctuations and nanodomains dynamics. Altogether, the four excitations explain the dielectric permittivity maximum in the kHz range