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Understanding the failure mechanisms of piezoelectric thin films is critical for the commercialization of piezoelectric microelectromechanical systems. This paper describes the failure of 0.6 mu m lead zirconate titanate (PZT) thin films on Si wafers with different in-plane stresses under large electric fields. The films failed by a combination of cracking and thermal breakdown events. It was found that the crack initiation and propagation behavior varied with the stress state of the films. The total stress required for crack initiation was estimated to be near 500 MPa. As expected, cracks propagated perpendicular to the maximum tensile stress direction. Thermal breakdown events and cracks were correlated, suggesting coupling between electrical and mechanical failure. It was also found that films that were released from the underlying substrates were less susceptible to failure by cracking. It was proposed that during electric field loading the released film stacks were able to bow and alleviate some of the stress. Released films may also experience enhanced domain wall motion that increases their fracture toughness. The results indicate that both applied stress and clamping conditions play important roles in the electromechancial failure of piezoelectric thin films. 

Many technologically critical materials are metastable under ambient conditions, yet the understanding of how to rationally design and guide the synthesis of these materials is limited. This work presents an integrated approach that targets a metastable lead‐free piezoelectric polymorph of SrHfO₃. First‐principles calculations predict that the previous experimentally unrealized, metastable P4mmphase of SrHfO₃should exhibit a direct piezoelectric response (d₃₃) of 36.9 pC N⁻¹(compared tod₃₃= 0 for the ground state). Combining computationally optimized substrate selection and synthesis conditions lead to the epitaxial stabilization of the polar P4mmphase of SrHfO₃on SrTiO₃. The films are structurally consistent with the theory predictions. A ferroelectric‐induced large signal effective converse piezoelectric response of 5.2 pm V⁻¹for a 35 nm film is observed, indicating the ability to predict and target multifunctionality. This illustrates a coupled theory‐experimental approach to the discovery and realization of new multifunctional polymorphs.