Enhanced dielectric response of ZrO2 upon Ti doping and introduction of O vacancies

We determine the electronic properties and dielectric response of zirconia (ZrO2) with oxygen vacancies (O vacancies) and Ti doping using first-principles density functional theory calculations based on pseudopotentials and a plane wave basis. We find significantly enhanced static dielectric response in zirconia with Ti doping and introduction of oxygen vacancies. Softening of phonon modes are responsible for the enhanced dielectric response of doped samples compared to pure zirconia.

Slim P‐E hysteresis loop and anomalous dielectric response in sol-gel derived antiferroelectric PbZrO3 thin films

Sol-gel derived PbZrO3 (PZ) thin films have been deposited on Pt(111)/Ti/SiO2/Si substrate and according to the pseudotetragonal symmetry of PZ, the relatively preferred (110)t oriented phase formation has been noticed. The room temperature P‐E hysteresis loops have been observed to be slim by nature. The slim hysteresis loops are attributed to the [110]t directional antiparallel lattice motion of Pb ions and by the directionality of the applied electric field. Pure PZ formation has been characterized by the dielectric phase transition at 235 °C and antiferroelectric P‐E hysteresis loops at room temperature. Dielectric response has been characterized within a frequency domain of 100 Hz–1 MHz at various temperatures ranging from 40 to 350 °C. Though frequency dispersion of dielectric behaves like a Maxwell–Wagner type of relaxation, ω2 dependency of ac conductivity indicates that there must be G‐C equivalent circuit dominance at high frequency. The presence of trap charges in PZ has been determined by Arrhenius plots of ac conductivity. The temperature dependent n (calculated from the universal power law of ac conductivity) values indicate an anomalous behavior of the trapped charges. This anomaly has been explained by strongly and weakly correlated potential wells of trapped charges and their behavior on thermal activation. The dominance of circuit∕circuits resembling Maxwell–Wagner type has been investigated by logarithmic Nyquist plots at various temperatures and it has been justified that the dielectric dispersion is not from the actual Maxwell–Wagner-type response.

Unusual dielectric response in B-site size-disordered hexagonal transition metal oxides

We discover that hexagonal holmium copper titanate (Ho2CuTiO6), has a unique and highly desirable combination of high dielectric constant, low losses, very small temperature coefficient, and low frequency dependence. Our first-principles calculations indicate that these exceptional properties result from a size-difference at the Cu/Ti B-site that suppresses the expected ferroelectric transition, combined with the dominance of intermediate-frequency polar vibrational modes in the dielectric response. Our results suggest that the use of such B-site disorder in alloys of hexagonal transition-metal oxides should generally result in similar robust dielectrics.

Dielectric response in pulsed laser ablated (Ba,Sr)TiO3 thin films

The dielectric response of pulsed laser ablated barium strontium titanate thin films were studied as a function of frequency and ambient temperature (from room temperature to 320 degrees C) by employing impedance spectroscopy. Combined modulus and impedance spectroscopic plots were used to study the response of the film, which in general may contain the grain, grain boundary, and the electrode/film interface as capacitive elements. The spectroscopic plots revealed that the major response was due to the grains, while contributions from the grain boundary or the electrode/film interface was negligible. Further observation from the complex impedance plot showed data points lying on a single semicircle, implying the response originated from a single capacitive element corresponding to the bulk grains. Conductivity plots against frequency at different temperatures suggested a response obeying the 'universal power law'. The value of the activation energies computed from the Arrhenius plots of both ac and dc conductivities with 1000/T were 0.97 and 1.04 eV, respectively. This was found to be in excellent agreement with published literature, and was attributed to the motion of oxygen vacancies within the bulk. (C) 2000 American Institute of Physics. [S0021-8979(00)02801-2].

High-temperature dielectric response in pulsed laser deposited Bi1.5Zn1.0Nb1.5O7 thin films

Cubic pyrochlore Bi1.5Zn1.0Nb1.5O7 thin films were deposited by pulsed laser ablation on Pt(200)/SiO2/Si at 500, 550, 600, and 650 degrees C. The thin films with (222) preferred orientation were found to grow at 650 degrees C with better crystallinity which was established by the lowest full-width half maxima of similar to 0.38. The dielectric response of the thin films grown at 650 degrees C have been characterized within a temperature range of 270-650 K and a frequency window of 0.1-100 kHz. The dielectric dispersion in the thin films shows a Maxwell-Wagner type relaxation with two different kinds of response confirmed by temperature dependent Nyquist plots. The ac conduction of the films showed a varied behavior in two different frequency regions. The power law exponent values of more than 1 at high frequency are explained by a jump-relaxation-model. The possibility of grain boundary related large polaronic hopping, due to two different power law exponents and transformation of double to single response in Nyquist plots at high temperature, has been excluded. The ``attempt jump frequency'' obtained from temperature dependent tangent loss and real part of dielectric constants, has been found to lie in the range of their lattice vibronic frequencies (10(12)-10(13) Hz). The activation energy arising from a large polaronic hopping due to trapped charge at low frequency region has been calculated from the ac conduction behavior. The range of activation energies (0.26-0.59. eV) suggests that the polaronic hopping at low frequency is mostly due to oxygen vacancies. (C) 2010 American Institute of Physics. doi:10.106311.3457335]

Effects of Zr and Ti doping on the dielectric response of CeO2: A comparative first-principles study

Zr doping in ceria (CeO2) results in enhanced static dielectric response compared to pure ceria. On the other hand, Ti doping in ceria keeps its dielectric constant unchanged. We use first-principles density functional theory calculations based on pseudopotentials and a plane wave basis to determine electronic properties and dielectric response of Zr/Ti-doped and oxygen-vacancy-introduced ceria. Softening of phonon modes is responsible for the enhancement in dielectric response of Zr-doped ceria compared to that of pure ceria. The ceria-zirconia mixed oxides should have potential use as high-k materials in the semiconductor industry. (c) 2010 Elsevier Ltd. All rights reserved.

Dielectric response of BaZrO3/BaTiO3 and SrTiO3/BaZrO3 superlattices

Dielectric materials with high tunability, low loss, and desired range of permittivity are an attractive class of materials for a variety of applications in microwave components such as tunable filters, phase shifters, antennas, etc. In this article, we have investigated the low frequency dielectric properties of BaZrO3/BaTiO3 and SrTiO3/BaZrO3 superlattices of varying modulation periods for the potential application toward electrically tunable devices. The dielectric response of the superlattices as a function of temperature revealed remarkable stability for both types of superlattices, with no observed dielectric anomalies within that range. Dielectric losses were also nominally low with minimal variation within the measured temperature range. Sufficiently high tunability of ∼ 40% was observed for the BaZrO3/BaTiO3 superlattices at the lowest individual layer thicknesses. In comparison, the SrTiO3/BaZrO3 superlattices showed a minimum tunability for lowest period structures. It showed maximum tunability of ∼ 20% at 10 kHz and room temperature at an intermediate dimension of 3.85 nm periodicity superlattice. The tunability value degraded with increasing as well as decreasing periodicities for the SrTiO3/BaZrO3 superlattices. The dielectric response has been explained on the basis of size effects, interlayer coupling between dissimilar materials, domain contribution, and depolarizing electric fields.

Effect of AC&DC field on the dielectric response of (Pb,La)TiO3 thin films

Lanthanum doped lead titanate thin films are the potential candidates for the capacitors, actuators and pyroelectric sensor applications due to their excellent dielectric, and ferroelectric properties. Lanthanum doped lead titanate thin films are grown on platinum coated Si substrates by excimer laser ablation technique. A broad diffused phase transition with the maximum dielectric permittivity (ϵmax) shifting to higher temperatures with the increase of frequency, along with frequency dispersion below Tc, which are the signatures of the relaxor like characteristics were observed. The dielectric properties are investigated from −60°C to 200°C with an application of different dc fields. With increasing dc field, the dielectric constant is observed to reduce and phase transition temperature shifted to higher temperature. With the increased ac signal amplitude of the applied frequency, the magnitude of the dielectric constant is increasing and the frequency dispersion is observed in ferroelectric phase, whereas in paraelectric phase, there is no dispersion has been observed. The results are correlated with the existing theories.

Effect of calcium stoichiometry on the dielectric response of CaCu3Ti4O12 ceramics

CaxCu3Ti4O12 (x=0.90, 0.97, 1.0, 1.1 and 1.15) polycrystalline powders with variation in calcium content were prepared via the oxalate precursor route. The structural, morphological and dielectric properties of the ceramics fabricated using these powders were studied using X-ray diffraction, scanning electron microscope along with energy dispersive X-ray analysis, transmission electron microscopy, electron spin resonance (ESR) spectroscopy and impedance analyzer. The X-ray diffraction patterns obtained for the x = 0.97, 1.0 and 1.1 powdered ceramics could be indexed to a body-centered cubic perovskite related structure associated with the space group Im3. The ESR studies confirmed the absence of oxygen vacancies in the ceramics that were prepared using the oxalate precursor route. The dielectric properties of these suggest that the calcium deficient sample (x = 0.97) has a reduced dielectric loss while retaining the high dielectric constant which is of significant industrial relevance. (C) 2012 Elsevier Ltd. All rights reserved.

Nonlinear dielectric response of BaBi4Ti4O15 ceramics

Nonlinear dielectric response of BaBi4Ti4O15 ceramics synthesized via the conventional solid-state reaction route has been monitored over a wide range of electric field strengths (E-0 = 0.5 - 5 kV/cm). Dielectric permittivity was found to increase linearly within the range of applied field. Rayleigh relations were employed to interpret the nonlinear dielectric response and the contribution of irreversible domain wall motion to the macroscopic permittivity was separated. The values of room temperature Rayleigh dielectric coefficient (alpha) and relative initial permittivity (epsilon'(init)) were found to be 2.28 +/- 0.02 cm/kV and 146.10 +/- 0.07, respectively. A reasonable agreement between the simulated and measured polarization-electric field (P-E) hysteresis loops was observed at an applied electric field of 5 kV/cm.

Glassy dielectric response in Tb2NiMnO6 double perovskite with similarities to a Griffiths phase

Results of frequency-dependent and temperature-dependent dielectric measurements performed on the double-perovskite Tb2NiMnO6 are presented. The real (epsilon(1)(f,T)) and imaginary (epsilon(2)(f,T)) parts of dielectric permittivity show three plateaus suggesting dielectric relaxation originating from the bulk, grain boundaries and the sample-electrode interfaces, respectively. The epsilon(1)(f,T) and epsilon(2)(f,T) are successfully simulated by a RC circuit model. The complex plane of impedance, Z'-Z `', is simulated using a series network with a resistor R and a constant phase element. Through the analysis of epsilon(f,T) using the modified Debye model, two different relaxation time regimes separated by a characteristic temperature, T*, are identified. The temperature variation of R and C corresponding to the bulk and the parameter alpha from modified Debye fit lend support to this hypothesis. Interestingly, the T* compares with the Griffiths temperature for this compound observed in magnetic measurements. Though these results cannot be interpreted as magnetoelectric coupling, the relationship between lattice and magnetism is markedly clear. We assume that the observed features have their origin in the polar nanoregions which originate from the inherent cationic defect structure of double perovskites. Copyright (C) EPLA, 2013

Colossal dielectric behavior of semiconducting Sr2TiMnO6 ceramics

Manganitelike double perovskite Sr2TiMnO6 (STMO) ceramics fabricated from the powders synthesized via the solid-state reaction route, exhibited dielectric constants as high as similar to 10(5) in the low frequency range (100 Hz-10 kHz) at room temperature. The Maxwell-Wagner type of relaxation mechanism was found to be more appropriate to rationalize such high dielectric constant values akin to that observed in materials such as KxTiyNi(1-x-y)O and CaCu3Ti4O12. The dielectric measurements carried out on the samples with different thicknesses and electrode materials reflected the influence of extrinsic effects. The impedance studies (100 Hz-10 MHz) in the 180-300 K temperature range revealed the presence of two dielectric relaxations corresponding to the grain boundary and the electrode. The dielectric response of the grain boundary was found to be weakly dependent on the dc bias field (up to 11 V/cm). However, owing to the electrode polarization, the applied ac/dc field had significant effect on the low frequency dielectric response. At low temperatures (100-180 K), the dc conductivity of STMO followed a variable range hopping behavior. Above 180 K, it followed the Arrhenius behavior because of the thermally activated conduction process. The bulk conductivity relaxation owing to the localized hopping of charge carriers obeyed the typical universal dielectric response.

Colossal dielectric behavior of semiconducting $Sr_{2}TiMnO_{6}$ ceramics

Manganitelike double perovskite Sr2TiMnO6 (STMO) ceramics fabricated from the powders synthesized via the solid-state reaction route, exhibited dielectric constants as high as similar to 10(5) in the low frequency range (100 Hz-10 kHz) at room temperature. The Maxwell-Wagner type of relaxation mechanism was found to be more appropriate to rationalize such high dielectric constant values akin to that observed in materials such as KxTiyNi(1-x-y)O and CaCu3Ti4O12. The dielectric measurements carried out on the samples with different thicknesses and electrode materials reflected the influence of extrinsic effects. The impedance studies (100 Hz-10 MHz) in the 180-300 K temperature range revealed the presence of two dielectric relaxations corresponding to the grain boundary and the electrode. The dielectric response of the grain boundary was found to be weakly dependent on the dc bias field (up to 11 V/cm). However, owing to the electrode polarization, the applied ac/dc field had significant effect on the low frequency dielectric response. At low temperatures (100-180 K), the dc conductivity of STMO followed a variable range hopping behavior. Above 180 K, it followed the Arrhenius behavior because of the thermally activated conduction process. The bulk conductivity relaxation owing to the localized hopping of charge carriers obeyed the typical universal dielectric response.

Dielectric properties of Poly(vinylidene fluoride)/CaCu3Ti4O12 composites

The possibility of obtaining relatively high dielectric constant polymer-ceramic composite by incorporating the giant dielectric constant material, CaCu3Ti4O12 (CCTO) in a Poly(vinylidene fluoride) (PVDF) polymer matrix by melt mixing and hot pressing process was demonstrated. The structure, morphology and dielectric properties of the composites were characterized using X-ray diffraction, Thermal analysis. scanning electron microscope, and impedance analyzer. The effective dielectric constant a(epsilon(eff)) of the composite increased with increase in the volume fraction of CCTO at all the frequencies(100 Hz-1 MHz) under study. The dielectric loss did not show any variation up to 40% loading of CCTO, but showed an increasing trend beyond 40%. The room temperature dielectric constant as high as 95 at 100 Hz has been realized for the composite with 55 vol.% of CCTO, which has increased to about 190 at 150 degrees C. Theoretical models like Maxwell's, Clausius-Mossotti, Effective medium theory, logarithmic law and Yamada were employed to rationalize the dielectric behaviour of the composite and discussed. (C) 2010 Published by Elsevier Ltd.

Dielectric properties of poly(vinylidene luoride)/CaCu3Ti4O12 nanocrystal composite thick films

The poly(vinylidene fluoride)/CaCu3Ti4O12 (CCTO) nanocrystal composite films (thickness approximate to 85 mu m) with relatively high dielectric permittivity (90 at 100 Hz) were prepared by the solution casting followed by spin coating technique. The structural, the microstructural and the dielectric properties of the composites were studied using X-ray diffraction, Scanning Electron Microscope, and Impedance analyzer respectively. The effective dielectric permittivity (e(eff)) of the composite increased with increase in the volume fraction of CCTO at all the frequencies (100 Hz to 1 MHz) under investigation. The room temperature dielectric permittivity which is around 90 at 100 Hz, has increased to about 290 at 125 degrees C (100 Hz). These results may be exploited in the development of high energy density capacitors.