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.

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