TY - JOUR AU - Lauren M Garten AU - Shyam S Dwaraknath AU - Julian Walker AU - John S Mangum AU - Paul F Ndione AU - Yoonsang Park AU - Daniel A Beaton AU - Venkatraman Gopalan AU - Brian P Gorman AU - Laura T Schelhas AU - Michael F Toney AU - SusanTrolier ‐McKinstry AU - Kristin A Persson AU - David S Ginley AB -

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 P4mm phase of SrHfO3 should exhibit a direct piezoelectric response (d33) of 36.9 pC N−1 (compared to d33 = 0 for the ground state). Combining computationally optimized substrate selection and synthesis conditions lead to the epitaxial stabilization of the polar P4mm phase of SrHfO3 on SrTiO3. The films are structurally consistent with the theory predictions. A ferroelectric‐induced large signal effective converse piezoelectric response of 5.2 pm V−1 for 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.

BT - Advanced Materials DA - 05/2018 DO - 10.1002/adma.201800559 IS - 25 LA - eng N2 -

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 P4mm phase of SrHfO3 should exhibit a direct piezoelectric response (d33) of 36.9 pC N−1 (compared to d33 = 0 for the ground state). Combining computationally optimized substrate selection and synthesis conditions lead to the epitaxial stabilization of the polar P4mm phase of SrHfO3 on SrTiO3. The films are structurally consistent with the theory predictions. A ferroelectric‐induced large signal effective converse piezoelectric response of 5.2 pm V−1 for 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.

PY - 2018 EP - 1800559 ST - Adv. Mater. T2 - Advanced Materials TI - Theory‐Guided Synthesis of a Metastable Lead‐Free Piezoelectric Polymorph VL - 30 SN - 0935-9648 ER -