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Register a new userBroadband dielectric spectroscopy of Ba(Zr,Ti)O3: dynamics of relaxors and diffuse ferroelectrics
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Broadband dielectric spectroscopy from Hz up to the infrared (IR) range and temperature interval 10-300 K was carried out for xBaZrO3-(1-x)BaTiO3 (BZT-x, x = 0.6, 0.7, 0.8) solid solution ceramics and compared with similar studies for x = 0, 0.2, 0.4, 1 ceramics published recently (Phys. Rev. B 86, 014106 (2012)). Rather complex IR spectra without appreciable mode softening are ascribed to Last-Slater transverse optic (TO) phonon eigenvector mixing and possible two-mode mixed crystal behavior. Fitting of the complete spectral range requires a relaxation in the 100 GHz range for all the samples. Below 1 GHz another relaxation appears, which is thermally activated and obeys the same Arrhenius behavior for all the relaxor BZT samples. The frequently reported Vogel-Fulcher behavior in BZT relaxors is shown to be an artifact of the evaluation from the permittivity or loss vs. temperature dependences instead of its evaluation from loss vs. frequency maxima. The relaxation is assigned to local hopping of the off-centered Ti4+ ions in the frozen BTO clusters, whose size is rather small and cannot grow on cooling. Therefore BZT is to be considered as a dipolar glass rather than relaxor ferroelectric.
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We investigated domain nucleation process in epitaxial Pb(Zr,Ti)O3 capacitors under a modified piezoresponse force microscope. We obtained domain evolution images during polarization switching process and observed that domain nucleation occurs at particular sites. This inhomogeneous nucleation process should play an important role in an early stage of switching and under a high electric field. We found that the number of nuclei is linearly proportional to log(switching time), suggesting a broad distribution of activation energies for nucleation. The nucleation sites for a positive bias differ from those for a negative bias, indicating that most nucleation sites are located at ferroelectric/electrode interfaces.
Heterostructures consisting of PbZr0.2Ti0.8O3 and PbZr0.4Ti0.6O3 films grown on a SrTiO3 (100) substrate with a SrRuO3 bottom electrode were prepared by pulsed laser deposition. Using the additional interface provided by the ferroelectric bilayer structure and changing the sequence of the layers, the dislocation content and domain patterns were varied. The resulting microstructure was investigated by transmission electron microscopy. Macroscopic ferroelectric measurements have shown a large impact of the formation of dislocations and the a/c domain structure on the ferroelectric polarization and dielectric constant. A thermodynamic analysis using the LANDAU-GINZBURG-DEVONSHIRE approach that takes into account the ratio of the thicknesses of the two ferroelectric layers and electrostatic coupling is used to describe the experimental data.
It has been considered that polar nanoregions in relaxors form at Burns temperature Td approx 600 K. High-temperature dielectric investigations of Pb(Mg1/3Nb2/3)O3 (PMN) and 0.7PMN-0.3PbTiO3 reveal, however, that the dielectric dispersion around 600 K appears due to the surface-layer contributions. The intrinsic response, analyzed in terms of the universal scaling, imply much higher Td or formation of polar nanoregions in a broad temperature range, while high dielectric constants manifest that polar order exists already at the highest measured temperatures of 800 K. The obtained critical exponents indicate critical behavior associated with universality classes typically found in spin glasses.
We investigated the time-dependent domain wall motion of epitaxial PbZr0.2Ti0.8O3 capacitors 100 nm-thick using modified piezoresponse force microscopy (PFM). We obtained successive domain evolution images reliably by combining the PFM with switching current measurements. We observed that domain wall speed (v) decreases with increases in domain size. We also observed that the average value of v, obtained under applied electric field (Eapp),showed creep behavior: i.e. <v> ~ exp(-E0/Eapp)^$mu$ with an exponent $mu$ of 0.9 $pm$ 0.1 and an activation field E0 of about 700 kV/cm.
Ferroelectric relaxors are complex materials with distinct properties. The understanding of their dielectric susceptibility, which strongly depends on both temperature and probing frequency, have interested researchers for many years. Here we report a macroscopic and phenomenological approach based on statistical modeling to investigate and better understand how the dielectric response of a relaxor depends on temperature. Employing the Maxwell-Boltzmann distribution and considering temperature dependent dipolar orientational polarizability, we propose a minimum statistical model and specific equations to understand and fit numerical and experimental dielectric responses versus temperature. We show that the proposed formula can successfully fit the dielectric response of typical relaxors, including Ba(Zr,Ti)O$_{3}$, Pb(Zn$_{1/3}$Nb$_{2/3}$)$_{0.87}$Ti$_{0.13}$O$_{3}$, and Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$-0.05Pb(Zr$_{0.53}$Ti$_{0.47}$)O$_{3}$, which demonstrates the general applicability of this approach.
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