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Ferroelectric films suffer from both aging and degradation under high ac‐field drive conditions due to loss of polarization with time. In this study, the roles of defect chemistry and internal electric fields on the long‐term stability of the properties of piezoelectric films were explored. For this purpose, lead zirconate titanate (PZT) films with a Zr/Ti ratio of 52/48 doped with Mn‐ (PMZT) or Nb‐ (PNZT) were deposited on Pt coated Si substrates by the sol‐gel method. It was demonstrated that the magnitude of the internal field is much higher in PMZT films compared to PNZT films after poling in the temperature range of 25‐200°C under an electric field of −240 kV/cm. The development of the internal field is thermally activated, with activation energies from 0.5 ± 0.06 to 0.8 ± 0.1 eV in Mn doped films and from 0.8 ± 0.1 to 1.2 ± 0.2 eV in Nb doped films. The different activation energies for imprint suggests that the physical mechanism underlying the evolution of the internal field in PMZT and PNZT films differs; the enhanced internal field upon poling is attributed to (a) alignment of oxygen vacancy—acceptor ion defect dipoles (,) in PMZT films, and (b) thermionic injection of electron charges and charge trapping in PNZT films. In either case, the internal field reduces back switching, enhances the remanent piezoelectric properties, and dramatically improves the aging behavior. PMZT films exhibited the greatest enhancement, with reduced high temperature (180°C) aging rates of 2%‐3%/decade due to improved stability of the poled state. In contrast, PNZT films showed significantly larger high temperature aging rates (15.5%/decade) in the piezoelectric coefficient, demonstrating that the fully poled state was not retained with time.

 

High-performance piezoelectrics benefit transducers and sensors in a variety of electromechanical applications.The materials with the highest piezoelectric chargecoefficients (d33) are relaxor-PbTiO3 crystals, which were discovered two decades ago. We successfully grew Sm-doped Pb(Mg1/3Nb2/3)O3-PbTiO3 (Sm-PMN-PT) single crystals with even higher d33 values ranging from 3400 to 4100 picocoulombs per newton, with variation below 20%over the as-grown crystal boule, exhibiting good property uniformity. We characterized the Sm-PMN-PTon the atomic scale with scanning transmission electron microscopy and made first-principles calculations to determine that the giant piezoelectric properties arise fromthe enhanced local structural heterogeneity introduced by Sm3+ dopants. Rare-earth doping is thus identified as a general strategy for introducing local structural heterogeneity in order to enhance the piezoelectricity of relaxor ferroelectric crystals.