ELECTRICAL PROPERTIES OF LEAD FERROTANTALATE CERAMICS

ABSTRACT

Perovskite structures with high dielectric constants and magnetic properties play an important role in micro- and optoelectronics and have numerous practical applications. Relaxor type ferroelectric ceramics PbFe_1/2Ta_1/2O₃ with perovskite structure was subject of present studies. Pyrochlore free lead ferrotantalate ceramics were produced by solid state technology from oxides. Low- and infra-low frequency studies of dielectric properties of PbFe_1/2Ta_1/2O₃ ceramics have revealed considerable infra-low frequency dispersion at temperatures above the temperature of maximum dielectric permittivity. The observed dispersion described by lemniscates is due to a considerable Maxwell-Wagner relaxation.     

Combined Experimental and Computational Methods Reveal the Evolution of Buried Interfaces during Synthesis of Ferroelectric Thin Films

Understanding interfaces between dissimilar materials is crucial to the development of modern technologies, for example, semiconductor–dielectric and thermoelectric–semiconductor interfaces in emerging electronic devices. However, the structural characterization of buried interfaces is challenging because many measurement techniques are surface sensitive by design. When interested in interface evolution during synthesis, the experimental challenges multiply and often necessitate in situ techniques. For solution‐derived lead zirconate titanate (PZT) ferroelectric thin films, the evolution of buried interfaces during synthesis (including dielectric–metal and metal–metal) is thought to dramatically influence the resultant dielectric and ferroelectric properties. In the present work, multiple experimental and computational methods are combined to characterize interface evolution during synthesis of ferroelectric PZT films on platinized Si wafers—including in situ X‐ray diffraction during thermal treatment, aberration‐corrected scanning transmission electron microscopy of samples quenched from various synthesis states, and calculations using density functional theory. Substantial interactions at buried interfaces in the PZT/Pt/Ti/SiO _x /Si heterostructure are observed and discussed relative to their role(s) in the synthesis process. The results prove that perovskite PZT nucleates directly from the platinum (111)‐oriented bottom electrode and reveal the roles of Pb and O diffusion and intermetallic Pt₃Pb and Pt₃Ti phases.     

Universal Polarization Switching Behavior of Disordered Ferroelectrics

Universal scaling features of polarization switching are established experimentally in rather different classes of disordered ferroelectrics: in well‐studied lead‐zirconate titanate (PZT) ferroelectrics, in recently synthesized Cu‐stabilized 0.94(Bi_1/2Na_1/2)TiO₃–0.06BaTiO₃ (BNT‐BT) relaxor ferroelectrics, and in classical organic ferroelectrics P(VDF‐TrFE). These scaling properties are explained by an extended concept of an inhomogeneous field mechanism (IFM) of polarization dynamics in ferroelectrics. Accordingly, disordered ferroelectrics exhibit a wide spectrum of characteristic switching times due to a statistical distribution of values of the local electric field. How this distribution can be extracted from polarization measurements is demonstrated. Generally, it is shown that the polarization response is primarily controlled by the statistical characteristics of disorder rather than by a temporal law of the local polarization switching.     

Studies of the Room‐Temperature Multiferroic Pb(Fe0.5Ta0.5)0.4(Zr0.53Ti0.47)0.6O3: Resonant Ultrasound Spectroscopy,Dielectric, and Magnetic Phenomena

Recently, lead iron tantalate/lead zirconium titanate (PZTFT) was demonstrated to possess large, but unreliable, magnetoelectric coupling at room temperature. Such large coupling would be desirable for device applications but reproducibility would also be critical. To better understand the coupling, the properties of all 3 ferroic order parameters, elastic, electric, and magnetic, believed to be present in the material across a range of temperatures, are investigated. In high temperature elastic data, an anomaly is observed at the orthorhombic mm2 to tetragonal 4mm transition, T_ot = 475 K, and a softening trend is observed as the temperature is increased toward 1300 K, where the material is known to become cubic. Thermal degradation makes it impossible to measure elastic behavior up to this temperature, however. In the low temperature region, there are elastic anomalies near ≈40 K and in the range 160–245 K. The former is interpreted as being due to a magnetic ordering transition and the latter is interpreted as a hysteretic regime of mixed rhombohedral and orthorhombic structures. Electrical and magnetic data collected below room temperature show anomalies at remarkably similar temperature ranges to the elastic data. These observations are used to suggest that the three order parameters in PZTFT are strongly coupled.     

Critical Property in Relaxor-PbTiO(3) Single Crystals --- Shear Piezoelectric Response

The shear piezoelectric behavior in relaxor-PbTiO(3) (PT) single crystals is investigated in regard to crystal phase. High levels of shear piezoelectric activity, d(15) or d(24) >2000 pC N(-1), has been observed for single domain rhombohedral (R), orthorhombic (O) and tetragonal (T) relaxor-PT crystals. The high piezoelectric response is attributed to a flattening of the Gibbs free energy at compositions proximate to the morphotropic phase boundaries, where the polarization rotation is easy with applying perpendicular electric field. The shear piezoelectric behavior of pervoskite ferroelectric crystals was discussed with respect to ferroelectric-ferroelectric phase transitions and dc bias field using phenomenological approach. The relationship between single domain shear piezoelectric response and piezoelectric activities in domain engineered configurations were given in this paper. From an application viewpoint, the temperature and ac field drive stability for shear piezoelectric responses are investigated. A temperature independent shear piezoelectric response (d(24), in the range of -50°C to O-T phase transition temperature) is thermodynamically expected and experimentally confirmed in orthorhombic relaxor-PT crystals; relatively high ac field drive stability (5 kV cm(-1)) is obtained in manganese modified relaxor-PT crystals. For all thickness shear vibration modes, the mechanical quality factor Qs are less than 50, corresponding to the facilitated polarization rotation.     

Direct Observation of Capacitor Switching Using Planar Electrodes

Ferroelectric polarization switching in epitaxial (110) BiFeO₃ films is studied using piezoresponse force microscopy of a model in‐plane capacitor structure. The electrode orientation is chosen such that only two active domain variants exist. Studies of the kinetics of domain evolution allows clear visualization of nucleation sites, as well as forward and lateral growth stages of domain formation. It is found that the location of the reverse‐domain nucleation is correlated with the direction of switching in a way that the polarization in the domains nucleated at an electrode is always directed away from it. The role of interface charge injection and surface screening charge on switching mechanisms is explored, and the nucleation is shown to be controllable by the bias history of the sample. Finally, the manipulation of domain nucleation through domain structure engineering is illustrated. These studies pave the way for the engineering and design of the ferroelectric device structures through control of individual steps of the switching process.     

Electric Field‐Induced Oxidation of Ferromagnetic/Ferroelectric Interfaces

Composite multiferroics are a new class of material where magneto‐electric coupling is achieved by creating an interface between a ferromagnetic and a ferroelectric compound. The challenge of understanding the chemical and magnetic properties of such interface is a key to achieve good magneto‐electric coupling. The unique possibilities offered by isotope sensitive techniques are used to selectively investigate the interface's chemistry and magnetism in Fe/BaTiO₃ and Fe/LiNbO₃ systems during the application of an electric field. With a large enough electric field, a strong oxidation of Fe is triggered, which creates a magnetically dead interface. This leads to an irreversible decrease of the magneto‐electric coupling properties. Material parameters are identified that determine under which electric field the interface may be modified. The results are confirmed on the two systems and are expected to be widespread in this new class of hybrid material.