SearcharxivSearch

arXiv subjects

J. Petzelt

Publications and source records attributed to J. Petzelt.

At least 19 recordsLinked to original sources

Giant dielectric permittivity in Nb-doped rutile crystals

Dielectric properties of Nb-doped (~1.5 at%) rutile single crystals were studied in the 10-300 K temperature range (at frequencies below the MHz range down to 0.3 K) in a broad frequency range, up to terahertz and infrared range, to understand the origin of its giant permittivity. The results were fitted, modelled and compared with those of the undoped rutile crystal measured in the terahertz and infrared ranges. The primary effect originates from the near-electrode depletion layer of lower conductivity compared to the bulk (surface barrier-layer capacitor effect), which causes a strong thermally activated relaxation in the MHz dielectric spectra. In the higher frequency range, the main difference between doped and undoped crystals is the presence of an overdamped microwave excitation (central mode) in the doped crystal for both polarizations, persisting down to 10 K and not thermally activated. This accounts for the previously reported permittivity increase, even at 2 K - where all lower-frequency relaxations are frozen - compared to undoped crystals. It also explains why our low-frequency permittivity at 0.3K exceeds the THz value. The origin of this excitation remains unclear and requires further investigations. Doping affects polar phonons only by slightly increasing their damping.

cond-mat.mtrl-sci

Infrared, terahertz, and microwave spectroscopy of the soft and central modes in Pb(Mg1/3Nb2/3)O3

From the new infrared (IR) reflectivity and time-domain terahertz (THz) spectra combined with available high-frequency dielectric data above the MHz range in a broad temperature range of 10-900 K, a full picture of the soft and central mode behavior in the classical relaxor ferroelectric Pb(Mg1/3Nb2/3)O3 (PMN) is suggested. A detailed comparison is given with the recent hyper-Raman spectroscopy data (Phys. Rev. Lett. 117, 155501 (2016)), and also with other available experiments based on inelastic light and neutron scattering. The closest agreement is with the hyper-Raman data, both techniques yield the same number of soft-mode components and the same high-temperature softening towards the temperature T* ~ 400 K. In addition to evaluation of the IR-THz data using fitting with standard factorized form of the dielectric function, we performed a successful fitting of the same data using the effective medium approach (EMA), originally based on the assumption that the mesoscopic structure of PMN consists of randomly oriented uniaxially anisotropic polar nanodomains (PNDs) with somewhat harder TO polar modes in the direction along the local PND dipole (Phys. Rev. Lett. 96, 027601 (2006)). Evaluation using the Bruggeman EMA modelling has been successfully applied in the entire investigated temperature range. These results suggest that the response perpendicular to the local dipole moment, at high temperatures induced by random fields rather than PNDs, undergoes a classical softening from high temperatures with permittivity obeying the Curie-Weiss law, eps_per = C/(T-Tc), C = 1.7 x 10^5 K and Tc = 380 K. Below the Burns temperature ~620 K, a GHz relaxation ascribed to flipping of the PNDs emerges from the soft mode response, slows down and broadens, remaining quite strong towards the cryogenic temperatures, where it can be assigned to fluctuations of the PND boundaries.

cond-mat.mtrl-sci

Broadband dielectric spectroscopy of Ba(Zr,Ti)O3: dynamics of relaxors and diffuse ferroelectrics

Broadband dielectric spectroscopy from Hz up to the infrared (IR) range and temperature interval 10-300 K was carried out for xBaZrO3-(1-x)BaTiO3 (BZT-x, x = 0.6, 0.7, 0.8) solid solution ceramics and compared with similar studies for x = 0, 0.2, 0.4, 1 ceramics published recently (Phys. Rev. B 86, 014106 (2012)). Rather complex IR spectra without appreciable mode softening are ascribed to Last-Slater transverse optic (TO) phonon eigenvector mixing and possible two-mode mixed crystal behavior. Fitting of the complete spectral range requires a relaxation in the 100 GHz range for all the samples. Below 1 GHz another relaxation appears, which is thermally activated and obeys the same Arrhenius behavior for all the relaxor BZT samples. The frequently reported Vogel-Fulcher behavior in BZT relaxors is shown to be an artifact of the evaluation from the permittivity or loss vs. temperature dependences instead of its evaluation from loss vs. frequency maxima. The relaxation is assigned to local hopping of the off-centered Ti4+ ions in the frozen BTO clusters, whose size is rather small and cannot grow on cooling. Therefore BZT is to be considered as a dipolar glass rather than relaxor ferroelectric.

cond-mat.mtrl-sci

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.

cond-mat.mtrl-sci

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.

cond-mat.mtrl-sci

Polar phonons in some compressively stressed epitaxial and polycrystalline SrTiO3 thin films

Several SrTiO3 (STO) thin films without electrodes processed by pulsed laser deposition, of thicknesses down to 40 nm, were studied using infrared transmission and reflection spectroscopy. The complex dielectric responses of polar phonon modes, particularly ferroelectric soft mode, in the films were determined quantitatively. The compressed epitaxial STO films on (100) La0.18Sr0.82Al0.59-Ta0.41O3 substrates (strain 0.9%) show strongly stiffened phonon responses, whereas the soft mode in polycrystalline film on (0001) sapphire substrate shows a strong broadening due to grain boundaries and/or other inhomogeneities and defects. The stiffened soft mode is responsible for a much lower static permittivity in the plane of the compressed film than in the bulk samples.

cond-mat.mtrl-sci

Grain Size Influence on Dynamics of Polar Nanoclusters in PMN-35%PT Ceramics: Broadband Dielectric and Infrared Spectra

Dielectric response e*(f,T) and polar phonon spectra of coarse grain (grain size ~ 4 mkm) and fine grain (grain size ~ 150 nm) ceramics of PbMg_(1/3)Nb_(2/3)O3-35%PbTiO3 were investigated at temperatures 10 - 900 K. e*(f,T) in coarse-grain ceramics exhibits relaxor behavior at high temperatures and a sharp anomaly at the ferroelectric phase transition. The fine-grain ceramics exhibit mainly relaxor ferroelectric behavior with a smaller dielectric constant. The difference is explained by different relaxational dynamics of polar nanoclusters, which appear to be more stabilized at high temperatures in the fine-grain ceramics by pinning at grain boundaries. Below Tc, the growth of ferroelectric domains is suppressed in fine-grain ceramics as supported also by a second harmonic generation. On the other hand, polar phonon frequencies and their temperature dependences are almost independent of the grain size, but the selection rules for the cubic symmetry are not obeyed and all phonons are split due to a locally broken symmetry by polar nanoregions and chemical disorder. The lowest-frequency polar phonon undergoes partial softening down to ~ 0.1 THz near Tc = 440 K in both ceramics, but the dielectric anomaly is caused predominantly by flipping and breathing of polar nanoclusters. Due to contribution of both the soft phonon mode and dielectric relaxations into the dielectric constant, the ferroelectric phase transition, which corresponds to the percolation threshold of the polar nanoregions into macroscopic domains, can be considered as a special case of crossover between the displacive and order-disorder type.

cond-mat.mtrl-sci

Magnetodielectric effect and optic soft mode behaviour in quantum paraelectric EuTiO3 ceramics

Infrared reflectivity and time-domain terahertz transmission spectra of EuTiO3 ceramics revealed a polar optic phonon at 6 - 300K, whose softening is fully responsible for the recently observed quantum paraelectric behaviour. Even if our EuTiO3 ceramics show lower permittivity than the single crystal due to a reduced density and/or small amount of secondary pyrochlore Eu2Ti2O7 phase, we confirmed the magnetic field dependence of the permittivity, also slightly smaller than in single crystal. Attempt to reveal the soft phonon dependence at 1.8K on the magnetic field up to 13T remained below the accuracy of our infrared reflectivity experiment.

cond-mat.mtrl-sci

Dielectric relaxation and polar phonon softening in relaxor ferroelectric PbMg_(1/3)Ta_(2/3)O_3

Relaxor ferroelectric PbMg_1/3Ta_2/3O_3 ceramics and thin films were investigated by means of broad-band dielectric, time-domain terahertz (THz) and Fourier-transform infrared (IR) spectroscopy in the frequency range 100 Hz - 90 THz at temperatures 100 - 490 K, the THz and IR spectra were studied from 20 to 900K. Diffused and strongly temperature dependent peak in the complex permittivity is caused by a dielectric relaxation due to the dynamics of polar clusters. The relaxation appears below Burns temperature T_d in the THz range, slows down on cooling through the microwave and MHz range and anomalously broadens. The shortest and longest relaxation times of the distribution of relaxation times follow Arrhenius and Vogel-Fulcher law, respectively. The degree of B-site order has only a small influence on the parameters of the dielectric relaxation and almost no influence on the phonon parameters. Below T_m ~ 180K, the distribution of relaxation frequencies becomes broader than our experimental spectral range and frequency independent dielectric losses develop below 100 GHz in the spectra. Although the macroscopic crystal structure is cubic, IR spectra give evidence about the lower local symmetry which can be assigned to the presence of polar clusters below T_d. Infrared spectra above T_d still reveal more modes than predicted by selection rules in the paraelectric phase of the Fm-3m space group so that we suggest selection rules which take into account chemical inhomogeneity in the beta''-perovskite sublattice.

cond-mat.mtrl-sci

Quantum paraelectric behavior of pyrochlore PMN

Pb_1.83Mg_0.29Nb_1.71O_6.39 (PMN) crystallizing in a cubic pyrochlore structure exhibits, as the first dielectrics with pyrochlore structure, typical feature of quantum paraelectrics - its permittivity continuously increases on cooling and levels off below ~ 30K, without any signature of a structural phase transition. Broad-band dielectric spectra do not show any dielectric dispersion in the real part of permittivity up to 8.8 GHz. THz and infrared spectra reveal a soft polar optic mode which is responsible for the temperature dependence of the permittivity. The leveling-off of the permittivity at low temperatures obeys the Barrett formula and the fitted vibrational zero-point energy 1/(2*k_B*T_1) corresponds to the measured soft mode frequency. The number of observed infrared phonons exceeds that predicted from the factor-group analysis which indicates that the structure is at least locally non-cubic.

cond-mat.mtrl-sci

Infrared and THz studies of polar phonons and improper magnetodielectric effect in multiferroic BFO3 ceramics

BFO3 ceramics were investigated by means of infrared reflectivity and time domain THz transmission spectroscopy at temperatures 20 - 950 K, and the magnetodielectric effect was studied at 10 - 300 K, with the magnetic field up to 9 T. Below 175 K, the sum of polar phonon contributions into the permittivity corresponds to the value of measured permittivity below 1 MHz. At higher temperatures, a giant low-frequency permittivity was observed, obviously due to the enhanced conductivity and possible Maxwell-Wagner contribution. Above 200 K the observed magnetodielectric effect is caused essentially through the combination of magnetoresistance and the Maxwell-Wagner effect, as recently predicted by Catalan (Appl. Phys. Lett. 88, 102902 (2006)). Since the magnetodielectric effect does not occur due to a coupling of polarization and magnetization as expected in magnetoferroelectrics, we call it improper magnetodielectric effect. Below 175 K the magnetodielectric effect is by several orders of magnitude lower due to the decreased conductivity. Several phonons exhibit gradual softening with increasing temperature, which explains the previously observed high-frequency permittivity increase on heating. The observed non-complete phonon softening seems to be the consequence of the first-order nature of the ferroelectric transition.

cond-mat.mtrl-sci

Ferroelectric Soft Modes in Ceramics and Films

Ferroelectric soft mode properties in ceramics and thin films are reviewed and compared with single crystals. In general, the permittivity in ceramics and thin films is markedly reduced compared to the single crystals mainly because of low-permittivity grain boundaries - dead layers - (sometimes also nano-cracks) present in the samples. In SrTiO3 and BaTiO3, this dielectric reduction is fully explained by stiffening of the soft mode frequency. In most other ferroelectrics, the soft mode accounts only partly for such a permittivity reduction, since the transition is only partially driven by the phonon mode softening. In these cases, additional relaxational dispersion below the optical phonon range (central mode) accounts for the main part of the dielectric anomaly near Tc. Influence of nano-cracks on reduced permittivity near Tc and related stiffening of the central mode is manifested in the antiferroelectric PbZrO3 ceramics.

cond-mat.mtrl-sci

Anisotropic dielectric function in polar nano-regions of relaxor ferroelectrics

The paper suggests to treat the infrared reflectivity spectra of single crystal perovskite relaxors as fine-grained ferroelectric ceramics: locally frozen polarization makes the dielectric function strongly anisotropic in the phonon frequency range and the random orientation of the polarization at nano-scopic scale requires to take into account the inhomogeneous depolarization field. Employing a simple effective medium approximation (Bruggeman symmetrical formula) to dielectric function describing the polar optic modes as damped harmonic oscillators turns out to be sufficient for reproducing all principal features of room temperature reflectivity of PMN. One of the reflectivity bands is identified as a geometrical resonance entirely related to the nanoscale polarization inhomogeneity. The approach provides a general guide for systematic determination of the polar mode frequencies split by the inhomogeneous polarization at nanometer scale.

cond-mat.mtrl-sci

Far-infrared soft mode behavior in PST thin films

Temperature dependences of the optic phonons in $\rm PbSc_{1/2}Ta_{1/2}O_3$ sol-gel films deposited on sapphire substrates were studied by means of Fourier transform far-infrared transmission spectroscopy in the temperature range 20-900\K. Four films displaying different B-site order with both ferroelectric and relaxor behavior were studied. In all cases the TO mode near 80\icm{} at 10\K{} softens on heating to $\approx$45\icm{} following the Cochran law with extrapolated critical temperature near 700\K{} (400\K{} above the temperature of dielectric maximum, $T_{\rm m}$), but above 600\K{} its frequency remains stabilized. It can be assigned to the A$_{1}$ component of the ferroelectric soft mode inside polar clusters which form below the Burns temperature near 700\K. In the ordered PST film another mode activates below T$_{m}$ in infrared spectra near 60\icm exhibiting also anomalous temperature dependence due to its coupling with the former mode. It is assigned to the A$_{1}$ component of the F$_{2g}$ Raman active mode. Central mode, which appears below the Burns temperature in the THz range, is assigned to the dynamics of polar clusters. It slows down on cooling and vanishes from our spectral range below $T_{\rm m}$. Another overdamped excitation assigned to the E component of the soft mode appears near 30\icm{} at low temperatures.

cond-mat.mtrl-sci

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.

cond-mat.mtrl-sci

High-temperature phase transitions in SrBi_2Ta_2O_9 film: a study by THz spectroscopy

Time-domain THz transmission experiment was performed on a $\rm SrBi_2Ta_2O_9$ film deposited on sapphire substrate. Temperatures between 300 and 923 K were investigated and complex permittivity spectra of the film were determined. The lowest frequency optic phonon near 28 cm$^{-1}$ reveals a slow monotonic decrease in frequency on heating with no significant anomaly near the phase transitions. We show that the dielectric anomaly near the ferroelectric phase transition can be explained by slowing down of a relaxational mode, observed in the THz spectra. A second harmonic generation signal observed in a single crystal confirms a loss of center of symmetry in the ferroelectric phase and a presence of polar clusters in the intermediate ferroelastic phase.

cond-mat.mtrl-sci

Dielectric spectra of a new relaxor ferroelectric system Ba2LnTi2Nb3O15 (Ln=La, Nd)

New relaxor ferroelectric system has been synthesized. BLTN exhibits a smeared maximum of permittivity, characteristic of classic relaxor behaviour, with a peak shift from 185 K at 100 Hz to 300 K at 1 GHz. BNTN undergoes a first order ferroelectric phase transition at 389 K and BLNTN exhibits both a ferroelectric phase transition at 274 K and relaxor behaviour at higher temperatures.

cond-mat.mtrl-sci

Lattice Dynamics in PMN

Lattice dynamics for five ordered PMN supercells were calculated from first principles by the frozen phonon method. Maximal symmetries of all supercells are reduced by structural instabilities. Lattice modes corresponding to these instabilities, equilibrium ionic positions, and infrared reflectivity spectra were computed for all supercells. Results are compared with our experimental data for a chemically disordered PMN single crystal.

cond-mat.mtrl-sci