@article{50f07da4c3734afda355471154100e8d,
title = "Theory-Guided Synthesis of a Metastable Lead-Free Piezoelectric Polymorph",
abstract = "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.",
author = "Garten, {Lauren M.} and Shyam Dwaraknath and Julian Walker and Mangum, {John S.} and Ndione, {Paul F.} and Yoonsang Park and Beaton, {Daniel A.} and Venkatraman Gopalan and Gorman, {Brian P.} and Schelhas, {Laura T.} and Toney, {Michael F.} and Susan Trolier-McKinstry and Persson, {Kristin A.} and Ginley, {David S.}",
note = "Funding Information: The authors would like to thank Sanjini Nanayakkara for helpful discussions. This work was funded by the Center for the Next Generation of Materials by Design, an U.S. Department of Energy, Office of Science EFRC under Contract No. DE-AC36-08GO28308 to NREL. Use of the Stanford Synchrotron Radiation Lightsource, SLAC National Accelerator Laboratory, was supported by the U.S. Department of Energy, Office of Basic Energy Sciences under Contract No. DE-AC02-76SF00515. Y.P., S.T.M. and V.G. acknowledge support for the Penn State NSF-MRSEC Center for Nanoscale Science, grant number DMR 1420620. J.W. and S.T.M. acknowledge the support of the Steward S. Flaschen Professorship (United States). The DFT theory was conducted by S.D. and K.A.P., Films were grown by L.G. and P.N., SHG was conducted by Y.P. and V.G., TEM and SAED was conducted by J.M. and B.G., Synchrotron XRD was conducted by L.S. and M.T., RSM-XRD was conducted by D.B., and the dielectric, piezoelectric and ferroelectric measurements were conducted by J.W., L.G., and S.T.M. The project was supervised by D.G., and K.A.P. and L.G. wrote the paper with support from all authors. The project was developed by L.G., D.G., S.D., and K.A.P. All authors approve of the final paper for submission. Publisher Copyright: {\textcopyright} 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim",
year = "2018",
month = jun,
day = "20",
doi = "10.1002/adma.201800559",
language = "English (US)",
volume = "30",
journal = "Advanced Materials",
issn = "0935-9648",
publisher = "Wiley-VCH Verlag",
number = "25",
}