弛豫铁电体介电可调性的研究

无铅弛豫铁电体具有较好的介电可调性,在顺电相有较大的介电常数和极小的损耗,因较大的优值而被广泛地用于微波器件.根据现有的介电可调性理论,通过参量的适当修正,对介电可调性的表达式做了合理的探讨,结论适用于处理实验结果.比较发现,在电场作用下顺电相保持不变的近似得出的结论与实验结果差距较大,而转化为铁电相与实验结果完全吻合.考虑外加电场和自发极化对弹性吉布斯自由能的修正,导出了高电场对介电常数的修正关系,与实验结果相符.提出了介电可调度的概念与计算公式,能够定量表示掺杂对介电可调性的影响.     

弛豫铁电体弥散相变的玻璃化特性研究

根据弛豫铁电材料在相变区域的介电弥散行为和玻璃化 液体材料在过冷状态下黏度与温度的行为所共同满足的Vogel-Fulcher 函数关系, 分析了施主替代钛酸钡系列陶瓷的缺陷补偿原理, 通过引入玻璃化液体的构型熵概念, 研究了弛豫铁电材料中钛阳离子缺陷作用势的温度关系, 得到了如下结论: 施主掺杂含量的增加导致了无序度的增加, 钛离子缺陷浓度的增大和平均极性区域尺寸的减小; 在构型熵满足Vogel-Fulcher 函数关系的条件下, 温度越低, 钛离子缺陷作用的范围越大, 极化区域也越大. 缺陷作用的范围随温度的变化导致了弛豫铁电材料的弥散性. 温度下降到一定程度, 冻结效应发生, 介电弥散现象消失.     

Anisotropic dielectric function in polar nanoregions of relaxor ferroelectrics

The Letter suggests treating 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 nanoscopic scale requires taking into account the inhomogeneous depolarization field. Employing a simple effective medium approximation (the Bruggeman symmetrical formula) turns out to be sufficient for reproducing all principal features of room temperature reflectivity of Pb(Mg(1/3)Nb(2/3))O3. 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 the nanometer scale.     

核壳结构对弛豫铁电体介电行为的影响

介电弥散和介电隔离率的温度非线性关系是弛豫铁电体的主要特征. 通过对掺杂成分以线性梯度递减的核壳结构进行热力学函数分析, 认为核壳结构能够在低温区保持较高的介电常数, 但不能导致介电隔离率与温度的非线性关系. 通过对不同浓度掺杂的铁电体扩散相变的比较, 认为掺杂浓度会影响晶粒掺杂成分的不均匀性, 在较宽的分布条件下会导致介电隔离率与温度的非线性关系. 因而在介电常数的峰值温度区域, 顺电相与铁电相的晶粒共存. 温度变化会影响两相比例及铁电畴的变化, 从而导致弛豫铁电体的介电弥散性. 核壳结构会增大介电弥散性. 铁电陶瓷的掺杂物种类、掺杂物浓度和烧结温度均会影响核壳结构的成分不均匀性和介电弥散性.     

Simulation on dielectric susceptibility and domain evolution of relaxor ferroelectrics

Dielectric susceptibility and domain evolution of the relaxor ferroelectrics have been simulated using the Monte Carlo method upon the Potts-Ising model. The grain size effect and the applied ac field frequency effect on the dielectric susceptibility were theoretically investigated. We found that the dielectric susceptibility increases and the T_m (the temperature at which the dielectric susceptibility reaches the maximum) shifts to lower temperature with increasing average grain size or decreasing frequency. In addition, we obtained the value of the relaxation parameter γ estimated from the linear fit of the modified Curie-Weiss law; its changing trend with increasing average grain size or increasing frequency was well consistent with the experimental observation. From the results of the domain pattern evolution process, we observed the differences between relaxor ferroelectrics and normal ferroelectrics subjected to an applied ac field.     

Monte Carlo simulation on dielectric relaxation and dipole cluster state in relaxor ferroelectrics

The Ginzburg--Landau theory on ferroelectrics with random field induced by dipole defects is studied by using Monte Carlo simulation, in order to investigate the dipole configuration and the dielectric relaxation of relaxor ferroelectrics. With the increase of random field, the dipole configuration evolves from the long-range ferroelectric order into the coexistence of short-range dipole-clusters and less polarized matrix. The dipole-cluster phase above the transition temperature and superparaelectric fluctuations far below this temperature are identified for the relaxor ferroelectrics. We investigate the frequency dispersion and the time-domain spectrum of the dielectric relaxation, demonstrating the Vogel--Fulcher relationship and the multi-peaked time-domain distribution of the dielectric relaxation.     

Slow polarization processes in relaxor ferroelectrics

The general features of the slow polarization kinetics in relaxor ferroelectrics, observed and studied by us in the specific example of crystals of barium-strontium niobate (SBN) solid solutions of various compositions and of lead magnesium niobate (PMN), are considered. The dielectric hysteresis loops and spectra of the polarization relaxation time distribution in quasi-static and static electric fields were found to reveal characteristic anomalies related to a random internal electric field in the bulk of a relaxor ferroelectric. Such a field caused by structural disorder accounts for the anomalously broad spectrum of potential barriers for domain walls. The part played by free charge carriers in the formation of giant barriers is demonstrated. The paper presents some quantitative data characterizing the specific features of the structure and physical properties of the relaxors.     

Measurement of landau coefficients in ferroelectrics using nonlinear dielectric spectroscopy

A method of measuring the phenomenological Landau-Ginzburg coefficients in an expansion of the free energy of ferroelectrics near the phase transition is proposed. This method is based on simultaneously recording five Fourier components of the current response to a sinusoidal voltage as a function of temperature. An analysis is made of a specific application of the method to Langmuir-Blodgett ultrathin ferroelectric films.     

Polarization-based adjustable memory behavior in relaxor ferroelectrics

The irreversible decay of the spontaneous polarization above the phase-transition temperature is a limiting factor in any application of ferroelectric crystals. Here we show that electric fields applied at high temperatures induce a preferred direction in the crystal which is stable even after repeated heating and cooling through the phase transition. This preference in direction leads to a reorientation of domains in the ferroelectric phase. We use pyroelectric measurements to show that the directional preference originates from internal charge carriers interacting with domain walls.     

Anomalies of polarization processes in relaxor ferroelectrics

The anomalous polarization of relaxor ferroelectrics (relaxors), such as solid solutions of barium-strontium niobate (SBN) and lead magnesium niobate (PMN), is studied in ac low-frequency (up to 10^?4 Hz) and dc electric fields. The results of studying dielectric hysteresis loops, polarization relaxation, the coercive-field distribution spectrum, nonlinear polarization for various scales of inhomogeneities, and polarization in a photosensitive SBN relaxor subjected to illumination are presented. All of the anomalous polarization properties of relaxors substantially distinguish them from ordinary homogeneous ferroelectrics and serve as signs and a measure of structural disorder. This article presents a brief review of our recent studies and some new results obtained as a result of their analysis.     

Investigation of nonlinear effects in glassy matter using dielectric methods

We summarize current developments in the investigation of glassy matter using nonlinear dielectric spectroscopy. This work also provides a brief introduction into the phenomenology of the linear dielectric response of glass-forming materials and discusses the main mechanisms that can give rise to nonlinear dielectric response in this material class. Here we mainly concentrate on measurements of the conventional dielectric permittivity at high fields and the higher-order susceptibilities characterizing the 3ω and 5ω components of the dielectric response as performed in our group. Typical results on canonical glass-forming liquids and orientationally disordered plastic crystals are discussed, also treating the special case of supercooled monohydroxy alcohols.     

Peculiarities of low- and infralow-frequency dielectric response of layered ferroelectrics

The low-and infralow-frequency dielectric properties of layered BaBi₂Nb₂O₉, Na_0.5Bi_8.5Ti₂Nb₄O₂₇, Na_0.5Bi_8.5Ti₂Ta₄O₂₇, and K_0.5Bi_8.5Ti₂Nb₄O₂₇ ferroelectrics have been investigated in a wide temperature range. Anomalies of the dielectric response of these materials have been found in the vicinity of 100°C; possible reasons for these anomalies are discussed.     

The lineshape of inelastic neutron scattering in relaxor ferroelectrics

We show that a microscopic reason for the steep drop of the optical phonon branch into an acoustic one (the so-called waterfall effect) in relaxor ferroelectrics may be the coupling of phonons with defects and impurities of different kinds, which is always present in relaxors. Namely, we do not specify the type of impurities but rather represent them as an ensemble of so-called two-level systems (TLS). This approach makes it possible to trace the evolution of the “waterfall” with temperature and the TLS concentration. To facilitate the planning of experiments on inelastic neutron scattering, we present a modification of the so-called Latin hypercube sampling method, which, based on some significance criteria, allows one to perform measurements that are highly significant for elucidating the physical nature of, e.g., phonon dispersion laws in relaxor ferroelectrics.     

Phase transition of ergodic space shrinking in succession and relaxor ferroelectrics

A special phase transition, the phase transition of ergodic space shrinking in succession (abbreviated as ES³ phase transition), is proposed according to the freezing process of the ordered microregion dipoles in relaxors. Its features are discussed. The special characteristics of relaxors are explained from the viewpoint of the ES³ phase transition.