Using a serial bilayer model we show that heterogeneous ferroelectric systems may exhibit substantial Maxwell–Wagner piezoelectric relaxation. The relaxation has its origin in the coupling of the dielectric and piezoelectric properties. The model predicts both retardation (positive phase angle and counterclockwise charge–pressure hysteresis) and relaxation (negative phase angle and clockwise charge–pressure hysteresis) of the longitudinal direct piezoelectric coefficient. The theoretical results are confirmed experimentally in ferroelectric ceramic–ceramic bilayers and in a single-phase ferroelectric Aurivillius compound ceramic in which neighboring grains with strongly anisotropic properties may behave as basic Maxwell–Wagner units.
Microstructure, structural defects, and piezoelectric response of bismuth titanate (Bi4Ti3O12)1−x and bismuth titanium niobate (Bi3TiNbO9)x solid solution with x=0.05 and 0.2 were investigated. Depending on x and on the sintering temperature different microstructures and piezoelectric responses were observed. For a low content in Bi3TiNbO9 (x=0.05) and a high sintering temperature (1130 °C), a coarse grain size is present, the number of structural defects within the grain is small, and there is a strong dependence of d33 on the ac pressure. For higher Bi3TiNbO9 (x=0.2) content or for lower sintering temperature (1080 °C) and x=0.05, the grain size is finer and a large number of structural defects is present within the grains. In particular, for x=0.2, high resolution transmission electron microscopy shows a high concentration of intergrowth defects which consist of Bi3TiNbO9 layers inserted in the Bi4Ti3O12 matrix in a more or less random way. In these samples, there is a very small dependence of d33 on the ac pressure and the piezoelectric hysteresis is likewise very small. The relation between microstructure and piezoelectric properties is discussed and it is shown that there is a good correlation between the dependence of the piezoelectric response on the ac pressure and the defect density. The piezoelectric response may be related to the structural defects present within the grain.
Hysteresis free and linear piezoelectric behavior of SrBi4Ti4O15 (SrBIT) is very promising for precise sensors/actuators devices. Despite a quite low longitudinal piezoelectric coefficient (around 15 pC/N), its elevated ferroelectric phase transition temperature (540°C) allows its use above 300°C. Electrical conductivity at such temperatures should be kept as low as possible in order to avoid loss of piezoelectric properties or charge drifts. Under reducing conditions, however, the electrical conductivity may change considerably. The electrical conductivity of SrBi4Ti4O15 (SrBIT) has been measured under controlled oxygen partial pressure at elevated temperatures (700-900°C) from 1 atm down to 10−15atm. From 1 atm down to 10−15 atm pO2, above 700°C, the conductivity of SrBIT exhibits a -1/4 slope in log-log scale indicating n-type conductivity and an impurity controlled oxygen vacancy concentration. A conductivity minimum is observed around 0.2 atm for undoped SrBIT at 800°C. Acceptor doping (Mn) raises the minimum and flattens the conductivity curve with slope around -1/10 at 700°C, and -1/6 at 900°C. Ionic conductivity and defect ionization are discussed to account for this. Preliminary results indicate the possibility of a large, pO2 independent, region, down to 10−15atm pO2. The ionic transport number was found to be 0.42 at 800°C for undoped SrBIT and 0.75 for Mn doped SrBIT. The activation energies of undoped (1.35 eV) and Mn doped (1.44 eV) samples are close to each other as expected for a common mechanism
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