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In view of serious environmental concerns with traditional Pb-based piezoelectrics, the search for new Pb-free alternatives has intensified recently. A thorough investigation of structure-property relationships in Pb-free piezoelectrics is desired in order to design new material compositions with high electromechanical properties that can be operated over a broader range of conditions. Recent availability of high-quality single crystals has not only opened the possibility for achieving multifold enhancements in the electromechanical properties in this new class of materials, but has also provided opportunities to undertake fundamental studies on their structure-property relationships. In the following pages, I review some of the recent X-ray and neutron diffraction studies of Pb-free piezoelectric single crystals, which have provided novel insights into their multiscale stimuli-induced structural mechanisms, including phase transitions, nanoscale structural ordering, lattice instability, and domain re-orientation. Opportunities and challenges for future progress in this area of study are discussed.

Characterization of Pb-Free KNbO3- and (Na,Bi)TiO3-Based Piezoelectric Single-Crystals Using X-ray and Neutron Diffraction