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Relaxor Behavior in Ordered Lead Magnesium Niobate (PbMg1/3Nb2/3O3) Thin Films

Journal Article · · Advanced Functional Materials
 [1];  [2];  [1];  [1];  [3];  [4];  [1]
  1. Pennsylvania State Univ., University Park, PA (United States). Dept. of Material Sciences and Engineering
  2. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering
  3. Pennsylvania State Univ., University Park, PA (United States). Dept. of Material Sciences and Engineering, Dept. of Physics, and Dept. of Engineering Science and Mechanics
  4. Univ. of California, Berkeley, CA (United States). Dept. of Materials Science and Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Materials Sciences Division
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The local compositional heterogeneity associated with the short-range ordering of Mg and Nb in PbMg1/3Nb2/3O3 (PMN) is correlated with its characteristic relaxor ferroelectric behavior. Fully ordered PMN is not prepared as a bulk material. This work examines the relaxor behavior in PMN thin films grown at temperatures below 1073 K by artificially reducing the degree of disorder via synthesis of heterostructures with alternate layers of Pb(Mg2/3Nb1/3)O3 and PbNbO3, as suggested by the random-site model. 100 nm thick, phase-pure films are grown epitaxially on (111) SrTiO3 substrates using alternate target timed pulsed-laser deposition of Pb(Mg2/3Nb1/3)O3 and PbNbO3 targets with 20% excess Pb. Selected area electron diffraction confirms the emergence of (1/2, 1/2, 1/2) superlattice spots with randomly distributed ordered domains as large as ≈150 nm. These heterostructures exhibit a dielectric constant of 800, loss tangents of ≈0.03 and 2× remanent polarization of ≈11 µC cm-2 at room temperature. Polarization–electric field hysteresis loops, Rayleigh data, and optical second-harmonic generation measurements are consistent with the development of ferroelectric domains below 140 K. Temperature-dependent permittivity measurements demonstrate reduced frequency dispersion compared to short range ordered PMN films. This research suggests a continuum between normal and relaxor ferroelectric behavior in the engineered PMN thin films.
Research Organization:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Organization:
National Science Foundation (NSF); US Army Research Office (ARO); USDOE Office of Science (SC)
Grant/Contract Number:
AC02-05CH11231
OSTI ID:
1637290
Journal Information:
Advanced Functional Materials, Journal Name: Advanced Functional Materials Journal Issue: 5 Vol. 29; ISSN 1616-301X
Publisher:
WileyCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
ferroelectricity
random site model
relaxor
short‐ and long‐range order
temperature‐dependent Rayleigh analysis