Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution

Jieun Kim, Hiroyuki Takenaka, Yubo Qi, Anoop R. Damodaran, Abel Fernandez, Ran Gao, Margaret R. McCarter, Sahar Saremi, Linh Chung, Andrew M. Rappe, Lane W. Martin

Research output: Contribution to journalArticlepeer-review

12 Scopus citations

Abstract

Understanding and ultimately controlling the large electromechanical effects in relaxor ferroelectrics requires intimate knowledge of how the local-polar order evolves under applied stimuli. Here, the biaxial-strain-induced evolution of and correlations between polar structures and properties in epitaxial films of the prototypical relaxor ferroelectric 0.68PbMg1/3Nb2/3O3–0.32PbTiO3 are investigated. X-ray diffuse-scattering studies reveal an evolution from a butterfly- to disc-shaped pattern and an increase in the correlation-length from ≈8 to ≈25 nm with increasing compressive strain. Molecular-dynamics simulations reveal the origin of the changes in the diffuse-scattering patterns and that strain induces polarization rotation and the merging of the polar order. As the magnitude of the strain is increased, relaxor behavior is gradually suppressed but is not fully quenched. Analysis of the dynamic evolution of dipole alignment in the simulations reveals that, while, for most unit-cell chemistries and configurations, strain drives a tendency toward more ferroelectric-like order, there are certain unit cells that become more disordered under strain, resulting in stronger competition between ordered and disordered regions and enhanced overall susceptibilities. Ultimately, this implies that deterministic creation of specific local chemical configurations could be an effective way to enhance relaxor performance.

Original languageEnglish (US)
Article number1901060
JournalAdvanced Materials
Volume31
Issue number21
DOIs
StatePublished - May 24 2019
Externally publishedYes

Bibliographical note

Funding Information:
J.K., H.T., and Y.Q. contributed equally to this work. This work was primarily funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE-AC02-05-CH11231 (Materials Project program KC23MP) for the development of the relaxor ferroelectric thin films. H.T. acknowledges support from the Office of Naval Research under grant N00014-17-1-2574. Y.Q. acknowledges support from the U.S. Department of Energy, Office of Basic Energy Sciences, under grant DE-FG02-07ER46431. A.R.D. acknowledges support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC-0012375 for the growth of ferroelectric materials. A.F. acknowledges support from the Army Research Office under grant W911NF-14-1-0104. R.G. acknowledges support from the National Science Foundation under grant OISE-1545907. M.R.M. acknowledges support from the Gordon and Betty Moore Foundation’s EPiQS Initiative, under grant GBMF5307. A.M.R. acknowledges support from the National Science Foundation under grant DMR-1719353. L.W.M. acknowledges support from the National Science Foundation under grant DMR-1708615. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The authors acknowledge computational support from the NERSC of the U.S. Department of Energy and the HPCMO of the U.S. Department of Defense.

Funding Information:
J.K., H.T., and Y.Q. contributed equally to this work. This work was primarily funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Materials Sciences and Engineering Division under Contract No. DE-AC02-05-CH11231 (Materials Project program KC23MP) for the development of the relaxor ferroelectric thin films. H.T. acknowledges support from the Office of Naval Research under grant N00014-17-1-2574. Y.Q. acknowledges support from the U.S. Department of Energy, Office of Basic Energy Sciences, under grant DE-FG02-07ER46431. A.R.D. acknowledges support from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, under Award Number DE-SC-0012375 for the growth of ferroelectric materials. A.F. acknowledges support from the Army Research Office under grant W911NF-14-1-0104. R.G. acknowledges support from the National Science Foundation under grant OISE-1545907. M.R.M. acknowledges support from the Gordon and Betty Moore Foundation's EPiQS Initiative, under grant GBMF5307. A.M.R. acknowledges support from the National Science Foundation under grant DMR-1719353. L.W.M. acknowledges support from the National Science Foundation under grant DMR-1708615. This research used resources of the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. The authors acknowledge computational support from the NERSC of the U.S. Department of Energy and the HPCMO of the U.S. Department of Defense.

Publisher Copyright:
© 2019 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim

Keywords

  • diffuse scattering
  • domain structure
  • polar nanodomains
  • relaxor ferroelectrics
  • strain control

Fingerprint Dive into the research topics of 'Epitaxial Strain Control of Relaxor Ferroelectric Phase Evolution'. Together they form a unique fingerprint.

Cite this