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Composites of triglycine sulfate (TGS) powder dispersed in a poly(vinylidene fluoride-trifluoroethylene) (P(VDF-TrFE), 70/30 mol%) copolymer matrix have been prepared using solvent casting followed by compression moulding. The composites have been characterized by means of scanning electron microscopy (SEM) and differential scanning calorimetry (DSC). Three groups of samples have been prepared: unpoled composites, composites with only the TGS phase poled and composites with both phases poled. The observed relative permittivity of these composites are consistent with the predictions of the Bruggeman model. When the TGS and copolymer phases are poled in the same direction, the piezoelectric activities of the two phases partially cancel each other while the pyroelectric activities reinforce. The pyroelectric coefficients exhibit good agreement with the effective-medium model. These composites have high pyroelectric figures of merit which increase as the volume fraction of TGS increases [ABSTRACT FROM AUTHOR]

We have investigated the effects of electrical conductivity of the constituents on the poling behavior, dielectric, pyroelectric and piezoelectric properties of ferroelectric 0-3 composites. Modeling of polarization behavior is explored for both dc and ac poling procedures. Simulated results show that, in addition to the poling schedule, conductivity plays an important role in the poling process. Calculations are carried out for the time dependent internal electric fields induced by an ac field in dielectric measurements, by modulated temperature in pyroelectric measurement or by stress in piezoelectric measurement. Our previously developed models for dielectricity, pyroelectricity and piezoelectricity have been extended to include the additional contribution from the electrical conductivities. These can be significant for ceramic/polymer composites possessing high conductivity in the matrix phase. Calculated values based on the new model are discussed and compared with the previous models, and in particular the pyroelectric activities reported in the literature for a graphite doped lead zirconate titanate / polyurethane composite. Explicit expressions for the transient and steady state responses are given and the effective permittivity, pyroelectric and piezoelectric coefficients are derived in this paper. Remarkable enhancement in these coefficients is obtained when higher conductivity is introduced in the matrix phase. [ABSTRACT FROM AUTHOR]

To elucidate the molecular origin of the polarization dynamics in the ferroelectric relaxor poly(vinylidene fluoride—trifluoroethylene-chlorofluoroethylene) (P(VDF-TrFE-CFE)) terpolymer, a broadband dielectric study was carried out in the frequency range from 0.01 Hz to 10 MHz and temperatures from −150?C to 120?C for the terpolymer and a normal ferroelectric P(VDF-TrFE) copolymer. The relaxation processes were also studied using dynamic mechanical analysis. It was shown that in the terpolymer, which was completely converted to a ferroelectric relaxor, there is no sign of the relaxation process associated with the ferroelectric-paraelectric transition which occurs in the P(VDF-TrFE) copolymer. In the copolymer, three additional relaxation processes have been observed. It was found that the relaxation process βa, which was commonly believed to be associated with the glass transition in the amorphous phase, in fact, contains significant contribution from chain segment motions such as domain boundary motions in the crystalline region. In the temperature range studied, the terpolymer exhibits the latter three relaxation processes with the one (termed βr) near the temperature range of βa significantly enhanced. This is consistent with the observation that in conversion from the normal ferroelectric to a ferroelectric relaxor, the macro-polar domains are replaced by nano-polar-clusters and the boundary motions as well as the reorientation of these nano-clusters generate the high dielectric response. The experimental data also reveal a broad relaxation time distribution related for the βr process whose distribution width increases with reduced temperature, reflecting the molecular level heterogeneity in the crystalline phase due to the random introduction of the CFE monomer in the otherwise ordered macro-polar domains. The random interaction among the nano-clusters as well as the presence of the random fields produces ferroelectric relaxor behavior in the terpolymer. [ABSTRACT FROM AUTHOR]

Three kinds of near-field microscopy imaging mode including SEAM (Scanning electron acoustic microscopy), PFM (Piezoresponse force microscopy) and SPAM (Scanning probe acoustic microscopy) have been developed to investigate domain structures of ferroelectric ceramics, crystals and thin films in our studies. The domain imaging mechanisms are presented individually in three imaging modes. Sub-surface micro-domain configuration of ferroelectric BaTiO3 ceramics and single crystal and their dynamic behavior under external fields were clearly visualized by SEAM. Ferroelectric domain structures of ferroelectric PZT thin film and PMN-PT single crystal were characterized by PFM. Nanoscale switching behavior and local field-induced nanoscale displacement behavior of domain structures in ferroelectric thin film were studied by PFM. Antiparallel domain patterns in ferroelectric transparent PLZT ceramics were also characterized by SPAM. The combination of SEAM, PFM and SPAM in application to imaging domain structures undoubtedly enrich our understanding of the nature of piezoelectricity and ferroelectricity at submicro-, even nano-meter scale [ABSTRACT FROM AUTHOR]

Heat generation is one of the significant problems in piezoelectrics for high power density applications. In this paper, we review the loss mechanisms in piezoelectrics first, followed by the heat generation processes for various drive conditions. Heat generation at off-resonance is caused mainly by dielectric loss tan δ′ (i.e., P-E hysteresis loss), not by mechanical loss, while the heat generation at resonance is mainly attributed to mechanical loss tan ′. Then, practical high power materials developed at Penn State is introduced, which exhibit the vibration velocity more than 1 m/s, leading to the power density capability 10 times of the commercially available "hard" PZTs. We propose a internal bias field model to explain the low loss and high power origin of these materials. Finally, using a low temperature sinterable "hard" PZT, we demonstrated a high power multilayer piezoelectric transformers [ABSTRACT FROM AUTHOR]

The goal of this research was the development of a portable therapeutic device for the treatment of diabetes. A 3×3 cymbal array has been successfully tested in noninvasive insulin delivery experiments. The cymbal is a composite flextensional transducer constructed from a poled PZT ceramic and shaped metal endcaps that amplify the transducer motions by two orders of magnitude. Nine cymbals are wired in parallel and potted in polyurethane to form the flat panel arrays. When driven near resonance (20 kHz), the array generated a low intensity acoustic beam of 100 mW/cm2. Animal experiments on hyperglycemic rats and rabbits demonstrated the ultrasonic enhancement of transdermal insulin delivery. [ABSTRACT FROM AUTHOR]

We review the most interesting aspects of the domain structure kinetics in ferroelectrics important for "domain engineering" and discuss them in the framework of a unified nucleation approach. In our approach the nucleation rate is determined by the local value of electric field produced not only by bound charges and voltage applied to the electrodes, but also by screening charges. As a result, any kinetically produced domain pattern, even being far from the equilibrium, can be stabilized by bulk screening. The domain evolution represents a self-organizing process in which the screening of polarization plays the role of feedback. The general approach was applied for the description of the domain kinetics in lithium niobate and lithium tantalate as the most versatile materials for applications. The revealed original scenarios of the domain structure evolution are attributed to the retardation of the screening processes. The decisive role of screening effectiveness for shapes of individual domains and scenarios of the sideways domain wall motion is demonstrated both experimentally and by computer simulation. The possibility to produce a self-assembled nano-scale domain structures with controlled periods has been shown [ABSTRACT FROM AUTHOR]

The last two decades have witnessed the proliferation piezoelectric composite transducers for an array of sensor and actuator applications. In this article, a concise summary of the major methods used in composite making, with special emphasis on Solid Freeform Fabrication (SFF), is provided. Fused Deposition of Ceramics (FDC) and Sanders Prototyping (SP) are two SFF techniques that have been utilized to make a variety of novel piezocomposites with connectivity patterns including (1-3), (3-2), (3-1), (2-2) and (3-3). The FDC technique has also been used to prototype a number of actuators such as tube arrays, spiral, oval, telescoping, and monomorph multi-material bending actuators. It has been demonstrated that SFF technology is a viable option for fabricating piezocomposite sensors and actuators with intricate geometry, unorthodox internal architecture, and complex symmetry. The salient aspects of processing of such composite sensors and actuators are summarized, and structure-processing-property relations are elaborated on. [ABSTRACT FROM AUTHOR]

The domain configuration and ferroelectric property of mode relaxor ferroelectrics (RFEs) are investigated by performing a two-dimensional Monte Carlo simulation based on the Ginzburg-Landau theory on ferroelectric phase transitions and the defect model as an approach to the electric dipole configuration in relaxor ferroelectrics. The evolution of domain pattern and domain wall configuration with lattice defect concentration and temperature is simulated, predicting a typical two-phase coexisted microstructure consisting of ferroelectric regions embedded in the matrix of a paraelectric phase. The diffusive ferroelectric transitions in terms of the spontaneous polarization hysteresis and dielectric susceptibility as a function of temperature and defect concentration are successfully revealed by the simulation, demonstrating the applicability of the defect model and the simulation algorithm. A qualitative consistency between the simulated results and the properties of proton-irradiated ferroelectric copolymer is presented [ABSTRACT FROM AUTHOR]

The low-fired high performance piezoelectric ceramics used for multilayer piezoelectric transformer were investigated. Based on the transient liquid phase sintering mechanism, by doping suitable eutectic additives and optimizing processing, the sintering temperature of the quaternary system piezoelectric ceramics with high piezoelectric properties could be lower to about 960-1000°C. The low-temperature sintering multilayer piezoelectric transformer (MPT) has been developed. Some characteristics of MPT were systemically studied. The measurements include the frequency response of input impedance, frequency response of phase difference between input voltage and current, frequency shifting with load, input impedance changing with load, phase difference between input voltage and current shifting with load, and phase difference between input voltage and vibration velocity. The vibration modes and resonance characters of MPT were measured by a Laser Doppler Scanning Vibrometer. Several kinds of MPT with high voltage step-up ratio, high power density, high transfer efficiency and low cost have been industrially produced and commercialized. It reveals a broad application prospect for back-light power of liquid crystal display and piezo-ionizer etc. [ABSTRACT FROM AUTHOR]

Advances in first-principles computational approaches have, over the past ten years, made possible the investigation of basic physical properties of simple ferroelectric systems. Recently, first-principles techniques also proved to be powerful methods for predicting finite-temperature properties of solid solutions in great details. Consequently, bulk perovskites are rather well understood nowadays. On the other hand, one task still remains to be accomplished by ab-initio methods, that is, an accurate description and a deep understanding of ferroelectric nanostructures. Despite the fact that nanometer scale ferroelectric materials have gained widespread interest both technologically and scientifically (partly because of novel effects arising in connection with the reduction of their spatial extension), first-principles-based calculations on ferroelectric nanostructures are rather scarce. For instance, the precise effects of the substrate, growth orientation, surface termination, boundary conditions and thickness on the finite-temperature ferroelectric properties of ultrathin films are not well established, since their full understandings require (i) microscopic insights on nanoscale behavior that are quite difficult to access and analyze via experimental probes, and (ii) the development of new computational schemes. One may also wonder how some striking features exhibited by some bulk materials evolve in the corresponding thin films. A typical example of such feature is the morphotropic phase boundary of various solid solutions, where unusual low-symmetry phases associated with a composition-induced rotation of the spontaneous polarization and an enhancement of dielectric and piezoelectric responses were recently discovered. In this paper, recent findings resulting from the development and use of numerical first-principles-based tools on ferroelectric ultrathin films are discussed [ABSTRACT FROM AUTHOR]

Substitutional charge disorder giving rise to quenched electric random-fields (RFs) is probably at the origin of the peculiar behavior of relaxor ferroelectrics, which are primarily characterized by their strong frequency dispersion of the dielectric response and by an apparent lack of macroscopic symmetry breaking at the phase transition. Spatial fluctuations of the RFs correlate the dipolar fluctuations and give rise to polar nanoregions in the paraelectric regime as has been evidenced by piezoresponse force microscopy (PFM) at the nanoscale. The dimension of the order parameter decides upon whether the ferroelectric phase transition is destroyed (e.g. in cubic PbMg1/3Nb2/3O3, PMN) or modified towards RF Ising model behavior (e.g. in tetragonal Sr1−xBaxNb2O6, SBN, x ≈ 0.4). Frustrated interaction between the polar nanoregions in cubic relaxors gives rise to cluster glass states as evidenced by strong pressure dependence, typical dipolar slowing-down and theoretically treated within a spherical random bond-RF model. On the other hand, freezing into a domain state takes place in uniaxial relaxors. While at Tc non-classical critical behavior with critical exponents ρ ≈ 1.8, β ≈ 0.1 and α ≈ 0 is encountered in accordance with the RF Ising model, below Tc ≈ 350 K RF pinning of the walls of frozen-in nanodomains gives rise to non-Debye dielectric response. It is relaxation- and creep-like at radio and very low frequencies, respectively. [ABSTRACT FROM AUTHOR]

The Laser Intensity Modulation Method (LIMM) is widely used for the determination of the spatial distribution of polarization in polar ceramics and polymers, and space charge in non-polar polymers. The analysis of experimental data requires a solution of a Fredholm integral equation of the 1st kind. This is an ill-posed problem that has multiple and very different solutions. One of the more frequently used methods of solution is based upon Tikhonov regularization. A new method, the Polynomial Regularization Method (PRM), was developed for solving the LIMM equation with an 8th degree polynomial using smoothing to achieve a stable and optimal solution. An algorithm based upon the L-curve method (LCM) was used for the prediction of the best regularization parameter. LIMM data were simulated for an arbitrary polarization distribution and were analyzed using PRM and LCM. The calculated distribution function was in good agreement with the simulated polarization distribution. Experimental polarization distributions in a poorly poled sample of polyvinylidene fluoride (PVDF) and in a LiNbO3 bimorph, and space charge in polyethylene were analyzed. The new techniques were applied to the analysis of 3-dimensional polarization distributions [ABSTRACT FROM AUTHOR]

Dielectric response of vinylidene fluoride type ferroelectric polymers is dominated by that of segmental motions in the amorphous phase in temperature range 200-300 K and contributions related to the local mode and ferroelectric-paraelectric transition in the crystalline phase of the polymer at higher temperatures. Diffuse and frequency-dependent dielectric anomaly observed in fast electron irradiated polyvinylidene fluoride-trifluoroethylene P(VDF/TrFE) has been related to relaxor-like behavior induced in the semicrystalline ferroelectric copolymers. As random field and the response of polar nanosize clusters determine the relaxor behavior the effects of disorder and fast electron irradiation (below and above TC) on the three contributions to the dielectric response of PVDF, P(VDF/TrFE)(75/25) and P(VDF/TrFE)(50/50) are shown. The processes involved in radiation-induced functionalization of PVDF-type polymers are discussed on the basis of results of ESR, IR and Raman spectroscopy studies [ABSTRACT FROM AUTHOR]

In this paper, we review recent advances in piezoresponse force microscopy (PFM) with respect to nanoscale ferroelectric research, summarize the basic principles of PFM, illustrate what information can be obtained from PFM experiments and delineate the limitations of PFM signal interpretation relevant to quantitative imaging of a broad range of piezoelectrically active materials. Particular attention is given to orientational PFM imaging and data interpretation as well as to electromechanics and kinetics of nanoscale ferroelectric switching in PFM. [ABSTRACT FROM AUTHOR]

The magnetoelectric (ME) effect of piezoelectric-magnetostrictive laminate composites, which is a product tensor, has been studied. Based on piezoelectric and piezomagnetic constituent equations, the longitudinal-mode vibration and equivalent circuits have been derived. The effective magnetoelectric coupling coefficient, voltage-gain, and output efficiency have been determined. Our results show: (i) that there is an extreme high voltage gain effect of >260 under resonance drive: the induced ME voltage is much higher than the input voltage to the coils for magnetic excitation; (ii) that there is an optimum ratio of the piezoelectric to piezomagnetic layer thicknesses, which results in maximum effective magnetoelectric coupling; and (iii) that the maximum output efficiency of magnetoelectric laminate at resonance drive is ∼98%, if eddy currents are neglected. This high ME voltage gain effect offers potential for power transformer applications [ABSTRACT FROM AUTHOR]

We have studied the relaxor behavior of sol-gel derived Ba(ZrxTi1−x)O3 (0.30≤x≤0.70) thin films. The plausible mechanism of the relaxor behavior has been analyzed from the dielectric data and micro-Raman spectra. Substitution of Zr+4 for Ti+4 in BaTiO3 lattice reduces its long-range polarization order yielding a diffused paraelectric to ferroelectric phase transition. The solid solution system is visualized as a mixture of Ti+4 rich polar region and Zr+4 rich regions and with the increase in Zr contents the volume fraction of the polar regions are progressively reduced. At about 25.0 at% Zr contents the polar regions exhibit typical relaxor behavior. The degree of relaxation increases with Zr content and maximizes at 40.0 at% Zr doped film. The frequency dependence of the polar regions follows Vogel-Fulcher relation with a characteristic cooperative freezing at freezing temperature (Tf). Below Tf, a long range polarization ordering was ascertained from the polarization hysteresis measurement [ABSTRACT FROM AUTHOR]

Frequency and phase agile microwave components such as tunable filters and phase shifters will require ferroelectric thin films that exhibit a nonlinear dependence of dielectric permittivity (ɛr) with dc electric bias, as well as a high material (Δɛr/tan δ) and device (or K-factor in phase shift/dB) figure of merits (FOM). Therefore, voltage tunable (Pb0.3Sr0.7)TiO3 (PST) thin films (90-150 nm) on (0001) sapphire were deposited by metalorganic chemical vapor deposition at rates of 10-15 nm/min. The as-deposited epitaxial PST films were characterized by Rutherford backscattering spectroscopy, X-ray methods, field emission scanning electron microscope, high resolution transmission electron microscopy, Raman spectroscopy, and electrical methods (7-17 GHz) using coplanar waveguide test structures. The epitaxial relationships were as follows: out-of-plane alignment of [111] PST//[0001] sapphire, and orthogonal in-plane alignments of $$ [1\bar 10] $$ PST//$$ [10\bar 10] $$ sapphire and $$ [\bar 1\bar 12] $$ PST//$$ [1\bar 210] $$ sapphire. The material FOM and device FOM (or K-factor) at 12 GHz were determined to be 632 and ∼13 degrees/dB, respectively. The results are discussed in light of the nanostructure and stress in epi-PST films. Finally, a rational basis for the selection of PST composition, substrate, and process parameters is provided for the fabrication of optimized coplanar waveguide (CPW) phase shifters with very high material and device FOMs. [ABSTRACT FROM AUTHOR]

This paper discusses the mechanisms that can contribute to the enhanced longitudinal piezoelectric effect along nonpolar directions in perovskite crystals, such as BaTiO3, PbTiO3, KNbO3, Pb(Mg1/3Nb2/3)O3-PbTiO3 and Pb(Zn1/2Nb2/3)O3-PbTiO3. Piezoelectric anisotropy is discussed in relation to temperature induced phase transitions, compositional variation in solid solutions with morphotropic phase boundaries, applied electric fields, the domain wall structure and domain wall displacement [ABSTRACT FROM AUTHOR]

After a brief historical introduction this article will present a summary of experimental work carried through at Penn State to explore the flexoelectric coefficients μijkl in ferroelectric, incipient ferroelectric and relaxor ferroelectric perovskites. The initial objective was to understand the magnitude of flexoelectricity in these systems to see whether it would be possible to develop a piezoelectric composite containing no piezoelectric element, which nonetheless could have practically useful properties. Recent discussions of the thermodynamic converse effect, ie. the generation of elastic strain by an electric field gradient, now suggest that such composites might be designed to have unique properties such as a direct but no converse effect, or vice-versa, and materials with this character could have important practical application. Present data already suggest that the direct effect may make an important contribution to the properties of epitaxial thin films where mismatch can give rise to very steep elastic strain gradients. Clearly, more work is needed to fully quantify the flexoelectric behavior. It will be important to measure single crystals in the ceramic systems which have been studied and to characterize the converse effect as a check of the measured values [ABSTRACT FROM AUTHOR]

Relaxor ferroelectrics were discovered almost 50 years ago among the complex oxides with perovskite structure. In recent years this field of research has experienced a revival of interest. In this paper we review the progress achieved. We consider the crystal structure including quenched compositional disorder and polar nanoregions (PNR), the phase transitions including compositional order-disorder transition, transition to nonergodic (probably spherical cluster glass) state and to ferroelectric phase. We discuss the lattice dynamics and the peculiar (especially dielectric) relaxation in relaxors. Modern theoretical models for the mechanisms of PNR formation and freezing into nonergodic glassy state are also presented [ABSTRACT FROM AUTHOR]

The central problem in the physics of relaxors is the nature of the polar nanoclusters. Whereas relaxors are homogeneous at high enough temperatures, polar nanoregions immersed in a neutral matrix are formed below a certain temperature Tb. This should lead to a two component system. Here we present direct microscopic evidence for the two component nature of relaxors. We show that the chemical shift perturbed 207Pb NMR spectra of these systems consist of an isotropic component corresponding to a spherical glassy matrix which does not respond to an applied electric field, and an anisotropic component, corresponding to frozen out polar nanoclusters which order in a strong enough electric field, forming a ferroelectric phase. This is as well reflected in the dynamic properties where the relaxation time distribution function starts to become asymmetric with decreasing temperature and a second maximum-which is never seen in dipolar glasses and is obviously due to polar clusters-appears on further cooling. We also show that the basic difference between dipolar glasses and relaxors is the fact that polar nanoclusters can be oriented in a strong enough electric field and a ferroelectric phase can be induced. This is not the case in dipolar glasses where the response is due to single dipoles which can not be ordered by applied electric fields. [ABSTRACT FROM AUTHOR]

Recent studies of the mechanism of piezoelectricity in PZT and related materials are reviewed and complemented by new analyses based on the Landau-Ginzburg-Devonshire theory of ferroelectricity. Particular attention is given to the nature of the morphotropic phase boundary between the tetragonal and rhombohedral perovskite phases and the accompanying peak in the piezoelectric coefficient. The importance of the changes in angular dependence of single crystal piezoelectric coefficients as a function of composition is highlighted together with the concept of field-induced rotation of the polarization in the (110) plane. It is shown that introducing the tendency to form monoclinic phases enhances this phenomenon. The model that the monoclinic phase in PZT is due to the condensation of local disorder in the polar cation displacements from the macroscopic tetragonal and rhombohedral phases is examined in some detail using statistical analyses of the Zr/Ti conformation. Whilst the concept of monoclinic nano-domains is not inconsistent with statistically random distributions, it is argued that some ordering of the B-site cations may be required to enable the transformation to a macroscopically observable phase. The implications of this model on the contribution of polarization rotation to piezoelectricity in PZT are discussed [ABSTRACT FROM AUTHOR]

Multifunctional ferroelectric materials offer a wide range of useful properties, from switchable polarization that can be applied in memory devices to piezoelectric and pyroelectric properties used in actuators, transducers and thermal sensors. At the nanometer scale, however, material properties are expected to be different from those in bulk. Fundamental problems such as the super-paraelectric limit, the influence of the free surface, and of interfacial and bulk defects on ferroelectric switching, etc., arise when scaling down ferroelectrics to nanometer sizes. In order to study these size effects, fabrication methods of high quality nanoscale ferroelectric crystals have to be developed. The present paper briefly reviews self-patterning and self-assembly fabrication methods, including chemical routes, morphological instability of ultrathin films, microemulsion, and self-assembly lift-off, employed up to the date to fabricate ferroelectric structures with lateral sizes in the range of few tens of nanometers. [ABSTRACT FROM AUTHOR]