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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:
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Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (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) (SC-22). 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:  
AC02-06CH11357; AC05-00OR22725
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, M. J., Gehring, P. M., Rosenkranz, S., Osborn, R., Ye, F., Liu, Y., Ruff, J. P. C., Chen, W., Wozniak, J. M., Luo, H., 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, M. J., Gehring, P. M., Rosenkranz, S., Osborn, R., Ye, F., Liu, Y., Ruff, J. P. C., Chen, W., Wozniak, J. M., Luo, H., 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, M. J., Gehring, P. M., Rosenkranz, S., Osborn, R., Ye, F., Liu, Y., Ruff, J. P. C., Chen, W., Wozniak, J. M., Luo, H., 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, M. J. and Gehring, P. M. and Rosenkranz, S. and Osborn, R. and Ye, F. and Liu, Y. and Ruff, J. P. C. and Chen, W. and Wozniak, J. M. and Luo, H. 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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