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Title: Theory-Guided Synthesis of a Metastable Lead-Free Piezoelectric Polymorph

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 paper presents an integrated approach that targets a metastable lead-free piezoelectric polymorph of SrHfO 3. First-principles calculations predict that the previous experimentally unrealized, metastable P4mm phase of SrHfO 3 should exhibit a direct piezoelectric response (d 33) of 36.9 pC N -1 (compared to d 33 = 0 for the ground state). Combining computationally optimized substrate selection and synthesis conditions lead to the epitaxial stabilization of the polar P4mm phase of SrHfO 3 on SrTiO 3. 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. Finally, this illustrates a coupled theory-experimental approach to the discovery and realization of new multifunctional polymorphs.
Authors:
ORCiD logo [1] ;  [2] ;  [3] ;  [4] ;  [1] ;  [3] ;  [1] ;  [3] ;  [4] ;  [5] ;  [6] ;  [3] ;  [7] ;  [1]
  1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States)
  3. Pennsylvania State Univ., University Park, PA (United States). Dept. of Materials Science and Engineering. Materials Research Inst.
  4. Colorado School of Mines, Golden, CO (United States)
  5. SLAC National Accelerator Lab., Menlo Park, CA (United States). Applied Energy Programs
  6. SLAC National Accelerator Lab., Menlo Park, CA (United States). Applied Energy Programs. Stanford Synchrotron Radiation Lightsource
  7. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
AC02-76SF00515; AC36-08GO28308; DMR 1420620; AC02-05CH11231
Type:
Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 25; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Research Org:
SLAC National Accelerator Lab., Menlo Park, CA (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States); Pennsylvania State Univ., University Park, PA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; lead-free piezoelectrics; metastability; theory-guided synthesis
OSTI Identifier:
1462358
Alternate Identifier(s):
OSTI ID: 1436813; OSTI ID: 1479418

Garten, Lauren M., Dwaraknath, Shyam, Walker, Julian, Mangum, John S., Ndione, Paul F., Park, Yoonsang, Beaton, Daniel A., Gopalan, Venkatraman, Gorman, Brian P., Schelhas, Laura T., Toney, Michael F., Trolier-McKinstry, Susan, Persson, Kristin A., and Ginley, David S.. Theory-Guided Synthesis of a Metastable Lead-Free Piezoelectric Polymorph. United States: N. p., Web. doi:10.1002/adma.201800559.
Garten, Lauren M., Dwaraknath, Shyam, Walker, Julian, Mangum, John S., Ndione, Paul F., Park, Yoonsang, Beaton, Daniel A., Gopalan, Venkatraman, Gorman, Brian P., Schelhas, Laura T., Toney, Michael F., Trolier-McKinstry, Susan, Persson, Kristin A., & Ginley, David S.. Theory-Guided Synthesis of a Metastable Lead-Free Piezoelectric Polymorph. United States. doi:10.1002/adma.201800559.
Garten, Lauren M., Dwaraknath, Shyam, Walker, Julian, Mangum, John S., Ndione, Paul F., Park, Yoonsang, Beaton, Daniel A., Gopalan, Venkatraman, Gorman, Brian P., Schelhas, Laura T., Toney, Michael F., Trolier-McKinstry, Susan, Persson, Kristin A., and Ginley, David S.. 2018. "Theory-Guided Synthesis of a Metastable Lead-Free Piezoelectric Polymorph". United States. doi:10.1002/adma.201800559.
@article{osti_1462358,
title = {Theory-Guided Synthesis of a Metastable Lead-Free Piezoelectric Polymorph},
author = {Garten, Lauren M. and Dwaraknath, Shyam and Walker, Julian and Mangum, John S. and Ndione, Paul F. and Park, Yoonsang and Beaton, Daniel A. and Gopalan, Venkatraman and Gorman, Brian P. and Schelhas, Laura T. and Toney, Michael F. and Trolier-McKinstry, Susan and Persson, Kristin A. and Ginley, David S.},
abstractNote = {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 paper 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. Finally, this illustrates a coupled theory-experimental approach to the discovery and realization of new multifunctional polymorphs.},
doi = {10.1002/adma.201800559},
journal = {Advanced Materials},
number = 25,
volume = 30,
place = {United States},
year = {2018},
month = {5}
}

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