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]
+ Show Author Affiliations
  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); 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)
OSTI Identifier:
1462358
Alternate Identifier(s):
OSTI ID: 1436813; OSTI ID: 1479418
Grant/Contract Number:  
AC02-76SF00515; AC36-08GO28308; DMR 1420620; AC02-05CH11231
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.
Copy to clipboard
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.
Copy to clipboard
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.
Copy to clipboard
@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}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
This content will become publicly available on May 10, 2019
Publisher's Version of Record
DOI:  10.1002/adma.201800559
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

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

Band theory and Mott insulators: Hubbard U instead of Stoner I
journal, July 1991

  • Anisimov, Vladimir I.; Zaanen, Jan; Andersen, Ole K.
  • Physical Review B, Vol. 44, Issue 3, p. 943-954
  • DOI: 10.1103/PhysRevB.44.943

Ab initiomolecular dynamics for liquid metals
journal, January 1993

    [ × clear filter / sort ]

    Similar records in OSTI.GOV collections: