DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: The relation of local order to material properties in relaxor ferroelectrics

Abstract

Correlating electromechanical and dielectric properties with nanometre-scale order is the defining challenge for the development of piezoelectric oxides. Current lead (Pb)-based relaxor ferroelectrics can serve as model systems with which to unravel these correlations, but the nature of the local order and its relation to material properties remains controversial. Here we employ recent advances in diffuse scattering instrumentation to investigate crystals that span the phase diagram of PbMg1/3Nb2/3O3-xPbTiO(3) (PMN-xPT) and identify four forms of local order. From the compositional dependence, we resolve the coupling of each form to the dielectric and electromechanical properties observed. We show that relaxor behaviour does not correlate simply with ferroic diffuse scattering; instead, it results from a competition between local antiferroelectric correlations, seeded by chemical short-range order, and local ferroic order. The ferroic diffuse scattering is strongest where piezoelectricity is maximal and displays previously unrecognized modulations caused by anion displacements. Our observations provide new guidelines for evaluating displacive models and hence the piezoelectric properties of environmentally friendly next-generation materials.

Authors:
 [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [4]; ORCiD logo [4];  [5];  [6];  [7];  [8]; ORCiD logo [1];  [6];  [3]
  1. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Northern Illinois Univ., DeKalb, IL (United States). Department of Physics
  2. National Inst. of Standards and Technology (NIST), Gaithersburg, MD (United States). NIST Center for Neutron Research
  3. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Neutron Scattering Division
  5. Cornell Univ., Ithaca, NY (United States). CHESS
  6. Simon Fraser University, Burnaby, British Columbia (Canada). Department of Chemistry and 4D LABS
  7. Argonne National Lab. (ANL), Argonne, IL (United States). Mathematics and Computer Science Division; Univ. of Chicago, IL (United States). Computation Institute
  8. Chinese Academy of Sciences, Shanghai (China). Shanghai Institute of Ceramics
Publication Date:
Research Org.:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22). Materials Sciences & Engineering Division; USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Science Foundation (NSF); US Department of the Navy, Office of Naval Research (ONR); Natural Sciences and Engineering Research Council of Canada (NSERC)
OSTI Identifier:
1474571
Alternate Identifier(s):
OSTI ID: 1465134
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Nature Materials
Additional Journal Information:
Journal Volume: 17; Journal Issue: 8; Journal ID: ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE

Citation Formats

Krogstad, Matthew J., Gehring, P. M., Rosenkranz, Stephen, Osborn, Raymond, Ye, Feng, Liu, Yaohua, Ruff, Jacob P. C., Chen, W., Wozniak, Justin M., Luo, Haosu, Chmaissem, O., Ye, Z. -G., and Phelan, D. The relation of local order to material properties in relaxor ferroelectrics. United States: N. p., 2018. Web. doi:10.1038/s41563-018-0112-7.
Krogstad, Matthew J., Gehring, P. M., Rosenkranz, Stephen, Osborn, Raymond, Ye, Feng, Liu, Yaohua, Ruff, Jacob P. C., Chen, W., Wozniak, Justin M., Luo, Haosu, Chmaissem, O., Ye, Z. -G., & Phelan, D. The relation of local order to material properties in relaxor ferroelectrics. United States. https://doi.org/10.1038/s41563-018-0112-7
Krogstad, Matthew J., Gehring, P. M., Rosenkranz, Stephen, Osborn, Raymond, Ye, Feng, Liu, Yaohua, Ruff, Jacob P. C., Chen, W., Wozniak, Justin M., Luo, Haosu, Chmaissem, O., Ye, Z. -G., and Phelan, D. Mon . "The relation of local order to material properties in relaxor ferroelectrics". United States. https://doi.org/10.1038/s41563-018-0112-7. https://www.osti.gov/servlets/purl/1474571.
@article{osti_1474571,
title = {The relation of local order to material properties in relaxor ferroelectrics},
author = {Krogstad, Matthew J. and Gehring, P. M. and Rosenkranz, Stephen and Osborn, Raymond and Ye, Feng and Liu, Yaohua and Ruff, Jacob P. C. and Chen, W. and Wozniak, Justin M. and Luo, Haosu and Chmaissem, O. and Ye, Z. -G. and Phelan, D.},
abstractNote = {Correlating electromechanical and dielectric properties with nanometre-scale order is the defining challenge for the development of piezoelectric oxides. Current lead (Pb)-based relaxor ferroelectrics can serve as model systems with which to unravel these correlations, but the nature of the local order and its relation to material properties remains controversial. Here we employ recent advances in diffuse scattering instrumentation to investigate crystals that span the phase diagram of PbMg1/3Nb2/3O3-xPbTiO(3) (PMN-xPT) and identify four forms of local order. From the compositional dependence, we resolve the coupling of each form to the dielectric and electromechanical properties observed. We show that relaxor behaviour does not correlate simply with ferroic diffuse scattering; instead, it results from a competition between local antiferroelectric correlations, seeded by chemical short-range order, and local ferroic order. The ferroic diffuse scattering is strongest where piezoelectricity is maximal and displays previously unrecognized modulations caused by anion displacements. Our observations provide new guidelines for evaluating displacive models and hence the piezoelectric properties of environmentally friendly next-generation materials.},
doi = {10.1038/s41563-018-0112-7},
journal = {Nature Materials},
number = 8,
volume = 17,
place = {United States},
year = {Mon Jun 25 00:00:00 EDT 2018},
month = {Mon Jun 25 00:00:00 EDT 2018}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record

Citation Metrics:
Cited by: 82 works
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Compositional dependence of structure, bulk properties and sources of diffuse scattering of PMN-xPT. a, Structural phase diagram for single crystals of PMN-xPT as adapted from ref. 16. 'SRO R/M' refers to a region in the phase diagram where there is short-range rhombohedral or monoclinic order that is resolvablemore » from the splitting of the fundamental Bragg reflections. 'Mc' refers to a monoclinic symmetry with space group Pm50. 'T' refers to tetragonal symmetry. b−f, Compositional dependence of various parameters. b, The piezoelectric coefficient, d33, as reported for single crystals and adapted from ref. 19. c, ΔTmax, as described in the main text. Data were collected and adapted from ref. 22. d, Amplitude of C1 measured with neutrons. Amplitude was estimated by integrating intensity over a section of the diffuse lobes around the 200 Bragg peak, centred on (2.14, 0.14, 0.0). e, Amplitude of the M-point scattering (C2), obtained by least-squares fitting of a Gaussian function to the (3.5, 0.5, 0.0) peak. f, Amplitude of the R-point scattering (C3) obtained by least-squares fitting of a Gaussian function to the (2.5, 0.5, 0.5) peak. g, Amplitude of the size-effect scattering (C4) obtained by integrating over a box of 0.4 × 0.4 × 0.4 reciprocal lattice units (r.l.u.) centred on (3.5, 0, 0). Linear vertical scales are used for d−g. Data were collected at 6 K for d−g.« less

Save / Share:

Works referenced in this record:

The giant electromechanical response in ferroelectric relaxors as a critical phenomenon
journal, June 2006


Recent progress in relaxor ferroelectrics with perovskite structure
journal, January 2006


Role of random electric fields in relaxors
journal, January 2014

  • Phelan, Daniel; Stock, Christopher; Rodriguez-Rivera, Jose A.
  • Proceedings of the National Academy of Sciences, Vol. 111, Issue 5
  • DOI: 10.1073/pnas.1314780111

Implementation of cross correlation for energy discrimination on the time-of-flight spectrometer CORELLI
journal, March 2018


Local Ordering in Lead-Based Relaxor Ferroelectrics
journal, June 2013

  • Goossens, Darren J.
  • Accounts of Chemical Research, Vol. 46, Issue 11
  • DOI: 10.1021/ar400073w

Effects of atomic short-range order on properties of the PbMg 1 / 3 Nb 2 / 3 O 3 relaxor ferroelectric
journal, November 2016


BZT: A Soft Pseudospin Glass
journal, November 2013


Relationship between Local Structure and Relaxor Behavior in Perovskite Oxides
journal, December 2007


The non-rhombohedral low-temperature structure of PMN–10% PT
journal, September 2004


Cold neutron study on the diffuse scattering and phonon excitations in the relaxor Pb ( Mg 1 3 Nb 2 3 ) O 3
journal, November 2004


Diffuse scattering in relaxor ferroelectrics: true three-dimensional mapping, experimental artefacts and modelling
journal, November 2011

  • Bosak, A.; Chernyshov, D.; Vakhrushev, Sergey
  • Acta Crystallographica Section A Foundations of Crystallography, Vol. 68, Issue 1
  • DOI: 10.1107/S0108767311040281

Anisotropic Local Correlations and Dynamics in a Relaxor Ferroelectric
journal, April 2013


Relaxor Pb ( Mg 1 / 3 Nb 2 / 3 ) O 3 : A Ferroelectric with Multiple Inhomogeneities
journal, November 2009


Glassy polarization behavior in ferroelectric compounds and
journal, December 1983


Damped soft phonons and diffuse scattering in 40 % Pb ( Mg 1 3 Nb 2 3 ) O 3 60 % PbTiO 3
journal, February 2006


Assessing Local Structure in PbZn1/3Nb2/3O3 Using Diffuse Scattering and Reverse Monte Carlo Refinement
journal, October 2012

  • Paściak, M.; Heerdegen, A. P.; Goossens, D. J.
  • Metallurgical and Materials Transactions A, Vol. 44, Issue 1
  • DOI: 10.1007/s11661-012-1475-z

Universal static and dynamic properties of the structural transition in Pb ( Zn 1 / 3 Nb 2 / 3 ) O 3
journal, March 2004


Diffuse phase transitions and random-field-induced domain states of the ‘‘relaxor’’ ferroelectric PbMg 1 / 3 Nb 2 / 3 O 3
journal, February 1992


X-ray and neutron diffraction studies of the diffuse phase transition in ceramics
journal, April 1991


Anti-ferrodistortive Nanodomains in PMN Relaxor
conference, January 2003

  • Tkachuk, A.
  • Fundamental Physics of Ferroelectrics 2003, AIP Conference Proceedings
  • DOI: 10.1063/1.1609938

A structural model for the relaxor PbMg 1/3 Nb 2/3 O 3 at 5 K
journal, October 1991


Evidence of decoupled lattice distortion and ferroelectric polarization in the relaxor system PMN x PT
journal, December 2003


Neutron and x-ray diffraction study of cubic [111] field-cooled Pb ( Mg 1 3 Nb 2 3 ) O 3
journal, August 2007


Mantid—Data analysis and visualization package for neutron scattering and μ SR experiments
journal, November 2014

  • Arnold, O.; Bilheux, J. C.; Borreguero, J. M.
  • Nuclear Instruments and Methods in Physics Research Section A: Accelerators, Spectrometers, Detectors and Associated Equipment, Vol. 764
  • DOI: 10.1016/j.nima.2014.07.029

Powder neutron diffraction study of phase transitions in and a phase diagram of ( 1 x ) [ Pb ( Mg 1 3 Nb 2 3 ) O 3 ] x Pb Ti O 3
journal, July 2006


Electric-field-induced redistribution of polar nano-regions in a relaxor ferroelectric
journal, January 2006

  • Xu, Guangyong; Zhong, Z.; Bing, Y.
  • Nature Materials, Vol. 5, Issue 2
  • DOI: 10.1038/nmat1560

Finite-Temperature Properties of Ba ( Zr , Ti ) O 3 Relaxors from First Principles
journal, June 2012


Diffuse Scattering from Lead-Containing Ferroelectric Perovskite Oxides
journal, January 2013


Diffuse neutron scattering in relaxor ferroelectric PbMg1/3Nb2/3O3
journal, January 2005

  • Vakhrushev, Sergey; Ivanov, Alexandre; Kulda, Jiri
  • Physical Chemistry Chemical Physics, Vol. 7, Issue 11
  • DOI: 10.1039/b416454g

Three-dimensional mapping of diffuse scattering in Pb ( Zn 1 3 Nb 2 3 ) O 3 x Pb Ti O 3
journal, November 2004


Expanding Lorentz and spectrum corrections to large volumes of reciprocal space for single-crystal time-of-flight neutron diffraction
journal, March 2016

  • Michels-Clark, Tara M.; Savici, Andrei T.; Lynch, Vickie E.
  • Journal of Applied Crystallography, Vol. 49, Issue 2
  • DOI: 10.1107/S1600576716001369

Do we need the Ether of Polar Nanoregions?
journal, April 2012


Soft phonon columns on the edge of the Brillouin zone in the relaxor PbMg 1 / 3 Nb 2 / 3 O 3
journal, June 2009


Synchrotron X-ray scattering study of lead magnoniobate relaxor ferroelectric crystals
journal, October 1996

  • Vakhrushev, S.; Nabereznov, A.; Sinha, S. K.
  • Journal of Physics and Chemistry of Solids, Vol. 57, Issue 10
  • DOI: 10.1016/0022-3697(96)00022-4

Corelli: Efficient single crystal diffraction with elastic discrimination
journal, October 2008


Neutron Diffuse Scattering in Lead-Based Relaxor Ferroelectrics and its Relationship to the Ultra-High Piezoelectricity
journal, April 2012


Effect of polar nanoregions on giant electrostriction and piezoelectricity in relaxor ferroelectrics
journal, June 2004


Neutron elastic diffuse scattering study of Pb ( Mg 1 / 3 Nb 2 / 3 ) O 3
journal, February 2004


Correlations between nanoscale chemical and polar order in relaxor ferroelectrics and the lengthscale for polar nanoregions
journal, August 2005


On short range ordering in the perovskite lead magnesium niobate
journal, August 1990

  • Hilton, A. D.; Barber, D. J.; Randall, C. A.
  • Journal of Materials Science, Vol. 25, Issue 8
  • DOI: 10.1007/BF00575371

Modeling of polar nanoregions dynamics on the dielectric response of relaxors
journal, June 2013

  • Ni, Y.; Chen, H. T.; Shi, Y. P.
  • Journal of Applied Physics, Vol. 113, Issue 22
  • DOI: 10.1063/1.4809977

Conformal Miniaturization of Domains with Low Domain-Wall Energy: Monoclinic Ferroelectric States near the Morphotropic Phase Boundaries
journal, November 2003


Relaxing with relaxors: a review of relaxor ferroelectrics
journal, April 2011


Single-crystal neutron diffuse scattering and Monte Carlo study of the relaxor ferroelectric PbZn 1/3 Nb 2/3 O 3 (PZN)
journal, July 2005

  • Welberry, T. R.; Gutmann, M. J.; Woo, Hyungje
  • Journal of Applied Crystallography, Vol. 38, Issue 4
  • DOI: 10.1107/S0021889805015918

The phase transition sequence and the location of the morphotropic phase boundary region in (1   x)[Pb (Mg 1/3 Nb 2/3 )O 3 ] xPbTiO 3 single crystal
journal, January 2003


Slush-like polar structures in single-crystal relaxors
journal, June 2017

  • Takenaka, Hiroyuki; Grinberg, Ilya; Liu, Shi
  • Nature, Vol. 546, Issue 7658
  • DOI: 10.1038/nature22068

The origin of ultrahigh piezoelectricity in relaxor-ferroelectric solid solution crystals
journal, December 2016

  • Li, Fei; Zhang, Shujun; Yang, Tiannan
  • Nature Communications, Vol. 7, Issue 1
  • DOI: 10.1038/ncomms13807

Anisotropic Local Correlations and Dynamics in a Relaxor Ferroelectric
text, January 2012


The role of random electric fields in relaxors
text, January 2014


Works referencing / citing this record:

Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution
journal, April 2019


Large Piezoelectricity in Ternary Lead‐Free Single Crystals
journal, November 2019

  • Wang, Yaojin; Luo, Chengtao; Wang, Shuhao
  • Advanced Electronic Materials, Vol. 6, Issue 1
  • DOI: 10.1002/aelm.201900949

Local atomic order and hierarchical polar nanoregions in a classical relaxor ferroelectric
journal, June 2019


Unexpectedly large energy variations from dopant interactions in ferroelectric HfO2 from high-throughput ab initio calculations
journal, December 2018

  • Falkowski, Max; Künneth, Christopher; Materlik, Robin
  • npj Computational Materials, Vol. 4, Issue 1
  • DOI: 10.1038/s41524-018-0133-4

Transparent ferroelectric crystals with ultrahigh piezoelectricity
journal, January 2020


Heterogeneous integration of single-crystalline complex-oxide membranes
journal, February 2020


Controllable anisotropic characteristics in solid solution ferroelectrics
journal, January 2019

  • Huang, Fei; Hu, Chengpeng; Tian, Hao
  • CrystEngComm, Vol. 21, Issue 45
  • DOI: 10.1039/c9ce01198f

K-space algorithmic reconstruction (KAREN): a robust statistical methodology to separate Bragg and diffuse scattering
journal, February 2020

  • Weng, James; Dill, Eric D.; Martin, James D.
  • Journal of Applied Crystallography, Vol. 53, Issue 1
  • DOI: 10.1107/s1600576719017060

Dielectric relaxation and local domain structures of ferroelectric PIMNT and PMNT single crystals
journal, October 2019

  • Li, Kai; Sun, Enwei; Qi, Xudong
  • Journal of the American Ceramic Society, Vol. 103, Issue 3
  • DOI: 10.1111/jace.16849

Promoting luminescence of Yb/Er codoped ferroelectric composite by polarization engineering for optoelectronic applications
journal, September 2019


Local atomic order and hierarchical polar nanoregions in a classical relaxor ferroelectric
journal, June 2019