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The design of core-shell materials affords additional degrees of freedom to tailor functional properties as compared to solid solution counterparts. Although to date most of the work in core-shell materials has focused on dielectrics, piezoelectric coreshell ceramics may gain similar interest. Generalities of core-shell functional ceramics features are addressed in this work. A model system, Bi 1/2 Na 1/2 TiO 3 -SrTiO 3 , is introduced to discuss structure-property relationships. We demonstrate that this system features a core-shell microstructure for the composition corresponding to 25 at.% Sr. The material is studied by means of macroscopic functional properties and in situ structural characterization techniques at different length scales, such as X-ray diffraction, transmission electron microscopy, and Raman spectroscopy. The evolution of the core-shell with field and temperature determines its functional properties. The high strain of the system, 0.3% at 4 kV/mm, is due to an electric-field-induced phase transition of the core and shell. Upon field removal the core remains in a poled state, whereas the shell is characterized by a reversible transformation. The reversibility of the phase transition of shells and associated switching are key features in the observed giant strain. Dielectric anomalies are found to be related to changes in oxygen octahedral tilting angles within the core and shell.

In 0.95[0.94Bi0.5Na0.5TiO3-0.06BaTiO3]-0.05CaTiO3 ceramics, the temperature TS (dielectric permittivity shoulder at about 125 °C) represents a transition between two different thermally activated dielectric relaxation processes. Below TS, the approximately linear decrease of the permittivity with the logarithm of frequency was attributed to the presence of a dominant ferroelectric phase. Above TS, the permittivity shows a more complicated dependence of the frequency and Raman modes indicate a sudden increase in the spatial disorder of the material, which is ascribed to the presence of a nonpolar phase and to a loss of interaction between polar regions. From 30 to 150 °C, an increase in the maximum polarization with increasing temperature was related to three possible mechanisms: polarization extension favoured by the simultaneous presence of polar and non-polar phases; the occurrence of electric field-induced transitions from weakly polar relaxor to ferroelectric polar phase; and the enhanced polarizability of the crystal structure induced by the weakening of the Bi-O bond with increasing temperature. The occurrence of different electric field induced polarization processes with increasing temperature is supported by the presence of additional current peaks in the current-electric field loops.

High-resolution x-ray diffraction (XRD), Raman spectroscopy and total scattering XRD coupled to atomic pair distribution function (PDF) analysis studies of the atomic-scale structure of archetypal BaZrxTi(1-x)O3 (x = 0.10, 0.20, 0.40) ceramics are presented over a wide temperature range (100-450 K). For x = 0.1 and 0.2 the results reveal, well above the Curie temperature, the presence of Ti-rich polar clusters which are precursors of a long-range ferroelectric order observed below TC. Polar nanoregions (PNRs) and relaxor behaviour are observed over the whole temperature range for x = 0.4. Irrespective of ceramic composition, the polar clusters are due to locally correlated off-centre displacement of Zr/Ti cations compatible with local rhombohedral symmetry. Formation of Zr-rich clusters is indicated by Raman spectroscopy for all compositions. Considering the isovalent substitution of Ti with Zr in BaZrxTi1-xO3, the mechanism of formation and growth of the PNRs is not due to charge ordering and random fields, but rather to a reduction of the local strain promoted by the large difference in ion size between Zr(4+) and Ti(4+). As a result, non-polar or weakly polar Zr-rich clusters and polar Ti-rich clusters are randomly distributed in a paraelectric lattice and the long-range ferroelectric order is disrupted with increasing Zr concentration.

Sodium bismuth titanate (NBT) ceramics are among the most promising lead-free materials for piezoelectric applications. This work reports the crystal structure and phase evolution of NBT and Fe-modified NBT (from 0-2 at% Fe) using synchrotron X-ray diffraction and Raman spectroscopy, both at ambient and elevated temperatures. The crystallographic results are discussed with reference to permittivity and piezoelectric thermal depolarization measurements of the same compositions. Changes in the depolarization temperature due to Fe substitution were detected by Raman spectroscopy, and were found to correlate closely with depolarization temperatures obtained from converse piezoelectric coefficient and permittivity measured in situ. The depolarization temperatures obtained from direct piezoelectric coefficient measured ex situ as well as the phase transition temperatures obtained from synchrotron X-ray diffraction were found to be at higher temperatures. The mechanisms underlying the relationship between permittivity and piezoelectric depolarization to structural transitions observed in Raman spectroscopy and X-ray diffraction are discussed.

Electrical energy storage systems (EESSs) with high energy density and power density are essential for the effective miniaturization of future electronic devices. Among different EESSs available in the market, dielectric capacitors relying on swift electronic and ionic polarization-based mechanisms to store and deliver energy already demonstrate high power densities. However, different intrinsic and extrinsic contributions to energy dissipations prevent ceramic-based dielectric capacitors from reaching high recoverable energy density levels. Interestingly, relaxor ferroelectric-based dielectric capacitors, because of their low remnant polarization, show relatively high energy density and thus display great potential for applications requiring high energy density properties. In this study, some of the main strategies to improve the energy density properties of perovskite lead-free relaxor systems are reviewed, including (i) chemical modification at different crystallographic sites, (ii) chemical additives that do not target lattice sites, and (iii) novel processing approaches dedicated to bulk ceramics, thick and thin films, respectively. Recent advancements are summarized concerning the search for relaxor materials with superior energy density properties and the appropriate choice of both composition and processing routes to match various applications’ needs. Finally, future trends in computationally-aided materials design are presented.

BaSnxTi1−xO3 solid solutions with compositions in the range x = 0–0.20 were studied by combining analysis of the field-induced dielectric and ferroelectric properties with Raman spectroscopic investigations. By combining techniques, the detection of specific features related to the ferroelectric-to-relaxor crossover with increasing Sn content is possible. Detailed tunability analysis of the x = 0.05 composition indicated that multiple components contribute to the dc-field induced permittivity response; these components are active in different temperature and field ranges and could be assigned to a few polarization mechanisms. First order reversal curves (FORC) for the material clearly show a transition from ferroelectric-to-relaxor behavior with increasing x, confirming the conclusions from the Raman and dielectric studies. This was evidenced by the shift of the FORC distribution over coercivities toward zero field values. Raman measurements allow the identification of the separate phases with varying Sn content and temperature, indicating large regions of phase coexistence. The composition x = 0.20 is in a predominantly relaxor state. This is ascribed to a large range of phase coexistence and to the presence of polar nanoregions promoted by Sn substitution on the B site of the perovskite unit cell ABO3.

Several PbZr 1−x Ti x O 3 (PZT) compositions in the proximity of the morphotropic phase boundary (MPB) were examined by means of Raman spectroscopy in the 15-800 K temperature range. Previous studies performed by other researchers using various techniques evidenced that, in the phase diagram of PZT, areas with rhombohedral/monoclinic and tetragonal/monoclinic phases coexist across the MPB. For these compositions, either long-range or short-range symmetry ordering of the monoclinic phase should be considered, so that no true rhombohedral-monoclinic-tetragonal phase boundary exists. In addition, the onset of antiferrodistortive phase transitions between high-T and low-T perovskite phases has been predicted by ab initio calculations and experimentally reported. In the present work, low-T and high-T Raman scattering spectra were collected on undoped PbZr 1−x Ti x O 3 with compositions x = 0.42, 0.45, 0.465, 0.48 and 0.53 in an attempt to clarify the current open issues on the phase diagram of PZT. Spectra clearly belonging to the respective phases were observed in the rhombohedral, monoclinic and tetragonal areas, thus confirming that monoclinic ordering is long-range only for a narrow range of compositions. Raman measurements at cryogenic temperatures allowed detecting all predicted low-T phases, including the tetragonal one. These results are in good agreement with both ab initio calculations and experimental results obtained by other authors on the same compositions.