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Title: Geometrical frustration and piezoelectric response in oxide ferroics

Abstract

Materials with increased functionality are often based on crystalline structures with significant local disorder. Typical examples are ferrroic oxides exhibiting large spontaneous polarization that can be rotated by an applied electric field, finding use in many important applications. Despite years of investigation, the exact structural origin of the increased piezoelectric response of oxide ferroics is still unclear. Frequently evoked models attribute it to emerging polar nanoregions inside a non-polar matrix, existence of a morphotropic boundary separating polar phases with different crystallographic symmetry, low-symmetry bridging phases facilitating polarization rotation, displacive and diffuse structural phase transitions. In this work we use both conventional and resonant high-energy x-ray diffraction coupled to atomic pair distribution function analysis and 3D computer simulations to examine the relationship between the local structure and piezoelectric properties of exemplary sodium-potassium niobate ferroics. We show that their increased piezoelectric response is primarily due to a geometrical frustration in the underlying perovskite lattice induced by local fluctuations in the tilt pattern of the constituent niobium-oxygen octahedra, and not to a crystal-crystal phase transition or distinct nanodomains. The fluctuations peak when the sodium to potassium ratio approaches one, leading to softening of the perovskite lattice and easing of polarization rotation under electricmore » field. Based on the experimental data and model calculations involving Goldschmidt's tolerance factor for the stability of perovskites, we also show that the fluctuations are driven by the mismatch between the radii of sodium and potassium atoms, and the increased piezoelectric response of sodium-potassium niobates indeed scales with the variance in the distribution of these radii about the average value. Thus we settle important aspects of the debate over the structure-piezoelectric property relationship for oxide ferroics, thereby providing a new perspective on the ongoing effort to improve their useful properties.« less

Authors:
ORCiD logo [1];  [2];  [2];  [3];  [4]
  1. Central Michigan Univ., Mount Pleasant, MI (United States)
  2. Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
  3. Virginia Tech India Center for Advanced Research and Education, Chennai, Tamil Nadu (India)
  4. Pennsylvania State Univ., University Park, PA (United States)
Publication Date:
Research Org.:
Central Michigan Univ., Mount Pleasant, MI (United States); Argonne National Lab. (ANL), Argonne, IL (United States). Advanced Photon Source (APS)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1594599
Alternate Identifier(s):
OSTI ID: 1582580
Grant/Contract Number:  
SC0006877; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 4; Journal Issue: 1; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Ferroelectricity; crystal structures; resonant high-energy XRD

Citation Formats

Petkov, Valeri, Kim, Jong-Woo, Shastri, Sarvjit, Gupta, Shashaank, and Priya, Shashank. Geometrical frustration and piezoelectric response in oxide ferroics. United States: N. p., 2020. Web. doi:10.1103/PhysRevMaterials.4.014405.
Petkov, Valeri, Kim, Jong-Woo, Shastri, Sarvjit, Gupta, Shashaank, & Priya, Shashank. Geometrical frustration and piezoelectric response in oxide ferroics. United States. doi:10.1103/PhysRevMaterials.4.014405.
Petkov, Valeri, Kim, Jong-Woo, Shastri, Sarvjit, Gupta, Shashaank, and Priya, Shashank. Mon . "Geometrical frustration and piezoelectric response in oxide ferroics". United States. doi:10.1103/PhysRevMaterials.4.014405.
@article{osti_1594599,
title = {Geometrical frustration and piezoelectric response in oxide ferroics},
author = {Petkov, Valeri and Kim, Jong-Woo and Shastri, Sarvjit and Gupta, Shashaank and Priya, Shashank},
abstractNote = {Materials with increased functionality are often based on crystalline structures with significant local disorder. Typical examples are ferrroic oxides exhibiting large spontaneous polarization that can be rotated by an applied electric field, finding use in many important applications. Despite years of investigation, the exact structural origin of the increased piezoelectric response of oxide ferroics is still unclear. Frequently evoked models attribute it to emerging polar nanoregions inside a non-polar matrix, existence of a morphotropic boundary separating polar phases with different crystallographic symmetry, low-symmetry bridging phases facilitating polarization rotation, displacive and diffuse structural phase transitions. In this work we use both conventional and resonant high-energy x-ray diffraction coupled to atomic pair distribution function analysis and 3D computer simulations to examine the relationship between the local structure and piezoelectric properties of exemplary sodium-potassium niobate ferroics. We show that their increased piezoelectric response is primarily due to a geometrical frustration in the underlying perovskite lattice induced by local fluctuations in the tilt pattern of the constituent niobium-oxygen octahedra, and not to a crystal-crystal phase transition or distinct nanodomains. The fluctuations peak when the sodium to potassium ratio approaches one, leading to softening of the perovskite lattice and easing of polarization rotation under electric field. Based on the experimental data and model calculations involving Goldschmidt's tolerance factor for the stability of perovskites, we also show that the fluctuations are driven by the mismatch between the radii of sodium and potassium atoms, and the increased piezoelectric response of sodium-potassium niobates indeed scales with the variance in the distribution of these radii about the average value. Thus we settle important aspects of the debate over the structure-piezoelectric property relationship for oxide ferroics, thereby providing a new perspective on the ongoing effort to improve their useful properties.},
doi = {10.1103/PhysRevMaterials.4.014405},
journal = {Physical Review Materials},
number = 1,
volume = 4,
place = {United States},
year = {2020},
month = {1}
}

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