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

Journal Article · · Nature Materials
 [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

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.

Research Organization:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
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)
Grant/Contract Number:
AC05-00OR22725; AC02-06CH11357
OSTI ID:
1474571
Alternate ID(s):
OSTI ID: 1465134
Journal Information:
Nature Materials, Vol. 17, Issue 8; ISSN 1476-1122
Publisher:
Springer Nature - Nature Publishing GroupCopyright Statement
Country of Publication:
United States
Language:
English
Citation Metrics:
Cited by: 82 works
Citation information provided by
Web of Science

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Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution journal April 2019
Large Piezoelectricity in Ternary Lead‐Free Single Crystals journal November 2019
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
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
Mechanisms underpinning the ultrahigh piezoelectricity in Sm-doped 0.705Pb(Mg 1/3 Nb 2/3 )O 3 -0.295PbTiO 3 : Temperature-induced metastable local structure and field-induced polarization rotation journal August 2019
K-space algorithmic reconstruction (KAREN): a robust statistical methodology to separate Bragg and diffuse scattering journal February 2020
Dielectric relaxation and local domain structures of ferroelectric PIMNT and PMNT single crystals journal October 2019
Promoting luminescence of Yb/Er codoped ferroelectric composite by polarization engineering for optoelectronic applications journal September 2019

Figures / Tables (11)