Dragan Damjanovic

Ferroelectric, dielectric and piezoelectric properties of ferroelectric thin films and ceramics

Ferroelectric, dielectric and piezoelectric properties of ferroelectric thin films and ceramics are reviewed with the aim of providing an insight into different processes which may affect the behaviour of ferroelectric devices, such as ferroelectric memories and micro-electro-mechanical systems. Taking into consideration recent advances in this field, topics such as polarization switching, polarization fatigue, effects of defects, depletion layers, and depolarization fields on hysteresis loop behaviour, and contributions of domain-wall displacement to dielectric and piezoelectric properties are discussed. An introduction into dielectric, pyroelectric, piezoelectric and elastic properties of ferroelectric materials, symmetry considerations, coupling of electro-mechanical and thermal properties, and definitions of relevant ferroelectric phenomena are provided.

Piezoelectric properties of Li- and Ta-modified (K0.5Na0.5)NbO3 ceramics

Lead-free, potassium sodium niobate piezoelectric ceramics substituted with lithium (K0.5−x∕2,Na0.5−x∕2,Lix)NbO3 or lithium and tantalum (K0.5−x∕2,Na0.5−x∕2,Lix)(Nb1−y,Tay)O3 have been synthesized by traditional solid state sintering. The compositions chosen are among those recently reported to show high piezoelectric properties [Y. Saito, H. Takao, T. Tani, T. Nonoyama, K. Takatori, T. Homma, T. Nagaya, and M. Nakamura, Nature (London) 42, 84 (2004); Y. Guo, K. Kakimoto, and H. Ohsato, Appl. Phys. Lett. 85, 4121 (2004); Mater. Lett. 59, 241 (2005)]. We show that high densities and piezoelectric properties can be obtained for all compositions by pressureless sintering in air, without cold isostatic pressing, and without any sintering aid or special powder treatment. Resonance and converse piezoelectric (strain-field) measurements show a thickness coupling coefficient kt of 53% and converse piezoelectric coefficient d33 around 200pm∕V for the Li-substituted ceramics, and a kt of 52% and d33 over 300pm∕V fo...

Origin of the large strain response in (K0.5Na0.5)NbO3-modified (Bi0.5Na0.5)TiO3-BaTiO3 lead-free piezoceramics

The mechanism of the giant unipolar strain recently observed in a lead-free piezoceramic, 0.92(Bi0.5Na0.5)TiO3−0.06BaTiO3−0.02(K0.5Na0.5)NbO3 [S.-T. Zhang, A. B. Kounga, E. Aulbach, H. Ehrenberg, and J. Rodel, Appl. Phys. Lett. 91, 112906 (2007) was investigated. The validity of the previously proposed mechanism that the high strain comes both from a significant volume change during the field-induced phase transition, from an antiferroelectric to a ferroelectric phase and the domain contribution from the induced ferroelectric phase was examined. Monitoring the volume changes from the simultaneously measured longitudinal and transverse strains on disk-shaped samples showed that the phase transition in this specific material does not involve any notable volume change, which indicates that there is little contribution from a volume change due to the phase transition to the total strain response. Temperature dependent hysteresis measurements on unpoled samples of a nearby ferroelectric composition, 0.93(Bi0.5...

Stress and frequency dependence of the direct piezoelectric effect in ferroelectric ceramics

It is shown that at weak alternating stress the relationship between the piezoelectrically induced charge and applied stress in ferroelectric ceramics has the same form as the Rayleigh law for magnetization versus magnetic field in ferromagnetic materials. Applicability of the Rayleigh law to the piezoelectric effect is demonstrated in detail for lead zirconate titanate (PZT) ceramics. Experimental results indicate that the dominant mechanism responsible for piezoelectric hysteresis and the dependence of the piezoelectric coefficient on the applied ac stress is the pinning of non-180° domain walls. The dependence of the piezoelectric coefficient on the frequency of the driving stress is examined and is shown to be due to the frequency dispersion of both reversible and irreversible components of domain-wall displacement. Analysis of the stress dependence of the piezoelectric phase angle reveals piezoelectric hysteresis contributions that are not necessarily due to Rayleigh-type displacement of domain walls...

A morphotropic phase boundary system based on polarization rotation and polarization extension

Many ferroelectric solid solutions exhibit enhanced electromechanical properties at the morphotropic boundary separating two phases with different orientations of polarization. The mechanism of properties enhancement is associated with easy paths for polarization rotation in anisotropically flattened free energy profile. Another mechanism of properties enhancement related to free energy flattening is polarization extension. It is best known at temperature-driven ferroelectric-paraelectric phase transitions and may lead to exceedingly large properties. Its disadvantage is temperature instability of the enhancement. In this paper a temperature-composition phase diagram is proposed that exhibits compositionally driven-phase transitions with easy paths for both polarization rotation and polarization extension.

Materials for high temperature piezoelectric transducers

The most significant advance in this field in the past year has been the demonstration that single-crystal langasite, La3Ga5SiO14, can be used, at least at high frequencies, at temperatures up to 1000 degrees C. New evidence suggests that domain-wall contributions to the piezoelectric response of bismuth-titanate-based high temperature ferroelectric ceramics may be controlled using suitably chosen dopants. Modified bismuth titanate compositions are interesting for sensor applications in the medium temperature range (up to 500 degrees C).

Contribution of the irreversible displacement of domain walls to the piezoelectric effect in barium titanate and lead zirconate titanate ceramics

The contribution from the irreversible displacement of non-180 degrees domain walls to the direct longitudinal piezoelectric d(33) coefficient of BaTiO3 and Pb(Zr,Ti)O-3 ceramics was determined quantitatively by using the Rayleigh law. Effects of the crystal structure and microstructure of the ceramics as well as the external d.c. pressure on the domain wall contribution to d(33) were examined. In barium titanate, this domain wall contribution is large (up to 35% of the total d(33), under the experimental conditions used) and dependent on the external d.c. pressure in coarse grained ceramics, and much smaller and independent of the external d.c. pressure in fine-grained samples. The presence of internal stresses in fine-grained ceramics could account for the observed behaviour. The analysis shows that the domain-wall contribution to the d(33) in lead zirconate titanate ceramics is large in compositions close to the morphotropic phase boundary that contain a mixture of tetragonal and rhombohedral phases, and in rhombohedral compositions (up to 40% of the total d(33)). The domain-wall contribution to the piezoelectric response from the irreversible displacement of domain walls is significantly smaller in tetragonal Pb(Zr,Ti)O-3 samples where it decreases with increasing spontaneous strain.

The Rayleigh law in piezoelectric ceramics

The direct longitudinal piezoelectric effect in lead zirconate titanate, barium titanate, bismuth titanate and strontium bismuth titanate ceramics was investigated with respect to the dependence on the amplitude of an alternating pressure. At low alternating pressure amplitudes, the behaviour of the piezoelectric charge and the piezoelectric coefficient may be explained in terms of the Rayleigh law originally discovered for magnetization and magnetic permeability in ferromagnetic materials. The charge versus pressure hysteresis loops measured for piezeoelectric ceramics may similarly be described as the Rayleigh loops. The results presented show that the Rayleigh law can be applied to irreversible displacement of several types of non- ferroelectric domain walls and imply universal validity of the Rayleigh law for displacement of ferromagnetic, ferroelastic and ferroelectric domain walls.

Piezoelectric properties of rhombohedral Pb(Zr, Ti)O3 thin films with (100), (111), and “random” crystallographic orientation

The longitudinal d33 piezoelectric coefficient was studied in rhombohedral Pb(Zr0.6Ti0.4)O3 thin films with (111), (100), and “random” orientation. The largest d33 was found in (100)-oriented films and the smallest along the polarization direction in (111)-oriented films. These results are in a good qualitative agreement with recent theoretical predictions [Du, Zheng, Belegundu, and Uchino, Appl. Phys. Lett. 72, 2421 (1998)]. The field dependence of d33 was also investigated as a function of crystallographic orientation of the films. It was found that (100)-oriented films with the highest piezoelectric coefficient exhibit the weakest nonlinearity. Observed variation in the piezoelectric nonlinearity with film orientation can be fully explained by taking into account domain-wall contributions, which are dependent on film orientation.

Evidence of domain wall contribution to the dielectric permittivity in PZT thin films at sub-switching fields

Through the use of relations analogous to that of the Rayleigh law, it is demonstrated that the ac electric field dependence of the permittivity of ferroelectric thin films can be described. It is further shown that both reversible and irreversible components of the permittivity decrease linearly with the logarithm of the frequency of the ac field. The results demonstrate that the models describing the interaction of domain walls and randomly distributed pinning centers in magnetic materials can be extended to the displacement of domain walls in ferroelectric thin films.