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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 Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (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. 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., and Phelan, D. Mon . "The relation of local order to material properties in relaxor ferroelectrics". United States. doi: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 = {2018},
month = {6}
}

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Cited by: 27 works
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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

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Works referenced in this record:

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Implementation of cross correlation for energy discrimination on the time-of-flight spectrometer CORELLI
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Effects of atomic short-range order on properties of the PbMg 1 / 3 Nb 2 / 3 O 3 relaxor ferroelectric
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BZT: A Soft Pseudospin Glass
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Relationship between Local Structure and Relaxor Behavior in Perovskite Oxides
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The non-rhombohedral low-temperature structure of PMN–10% PT
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Cold neutron study on the diffuse scattering and phonon excitations in the relaxor Pb ( Mg 1 3 Nb 2 3 ) O 3
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Diffuse scattering in relaxor ferroelectrics: true three-dimensional mapping, experimental artefacts and modelling
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    Works referencing / citing this record:

    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

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


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


    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

    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

    Anti-ferrodistortive Nanodomains in PMN Relaxor
    conference, January 2003

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

    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

    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


    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

    Glassy polarization behavior in ferroelectric compounds and
    journal, December 1983


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


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


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


    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

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


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


    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

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


    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

    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

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


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


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


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


    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

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


    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


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


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


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


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


    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

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


    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

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


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


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


    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


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


    BZT: A Soft Pseudospin Glass
    journal, November 2013


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


    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
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    • DOI: 10.1107/s0021889805015918

    The origin of ultrahigh piezoelectricity in relaxor-ferroelectric solid solution crystals
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    • Li, Fei; Zhang, Shujun; Yang, Tiannan
    • Nature Communications, Vol. 7, Issue 1
    • DOI: 10.1038/ncomms13807

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


    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


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