skip to main content
OSTI.GOV title logo U.S. Department of Energy
Office of Scientific and Technical Information

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 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:
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)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22); National Science Foundation (NSF)
OSTI Identifier:
1462358
Alternate Identifier(s):
OSTI ID: 1436813
Grant/Contract Number:  
AC02-76SF00515; AC36-08GO28308; DMR 1420620
Resource Type:
Journal Article: Accepted Manuscript
Journal Name:
Advanced Materials
Additional Journal Information:
Journal Volume: 30; Journal Issue: 25; Journal ID: ISSN 0935-9648
Publisher:
Wiley
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; lead-free piezoelectrics; metastability; theory-guided synthesis

Citation Formats

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., 2018. 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. Thu . "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 = {Thu May 10 00:00:00 EDT 2018},
month = {Thu May 10 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 10, 2019
Publisher's Version of Record

Save / Share:

Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Projector augmented-wave method
journal, December 1994


Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996


From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999


Electron-energy-loss spectra and the structural stability of nickel oxide: An LSDA+U study
journal, January 1998

  • Dudarev, S. L.; Botton, G. A.; Savrasov, S. Y.
  • Physical Review B, Vol. 57, Issue 3, p. 1505-1509
  • DOI: 10.1103/PhysRevB.57.1505

Ab initiomolecular dynamics for liquid metals
journal, January 1993