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Title: Oxygen-Vacancy-Induced Polar Behavior in (LaFeO 3) 2/(SrFeO 3) Superlattices

Complex oxides displaying ferroelectric and/or multiferroic behavior are of high fundamental and applied interest. In this work, for the first time, we show that it is possible to achieve polar order in a superlattice made up of two nonpolar oxides by means of oxygen vacancy ordering. Using scanning transmission electron microscopy imaging, we show the polar displacement of magnetic Fe ions in a superlattice of (LaFeO 3) 2/(SrFeO 3) grown on a SrTiO 3 substrate. Using density functional theory calculations, we systematically study the effect of epitaxial strain, octahedral rotations, and surface terminations in the superlattice and find them to have a negligible effect on the antipolar displacements of the Fe ions lying in between SrO and LaO layers of the superlattice (i.e., within La 0.5Sr 0.5FeO 3 unit cells). The introduction of oxygen vacancies, on the other hand, triggers a polar displacement of the Fe ions. We confirm this important result using electron energy loss spectroscopy, which shows partial oxygen vacancy ordering in the region where polar displacements are observed and an absence of vacancy ordering outside of that area.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5] ;  [5] ;  [5] ;  [6] ;  [1] ;  [7]
  1. Vanderbilt Univ., Nashville, TN (United States). Dept. of Physics and Astronomy; Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Korea Basic Science Inst., Daejeon (Korea). Division of Electron Microscopic Research
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division; Univ. Complutense Madrid (Spain). Complex Materials Physics Group
  4. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division; Korea Inst. of Science and Technology, Seoul (Korea). Electronic Materials Research Center
  5. Argonne National Lab. (ANL), Argonne, IL (United States). Materials Science Division
  6. Univ. of Tennessee, Knoxville, TN (United States). Dept. of Materials Science and Engineering
  7. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Materials Science & Technology Division
Publication Date:
Grant/Contract Number:
AC02-06CH11357; FG02-09ER46554; AC02-05CH11231; 239739; AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Nano Letters
Additional Journal Information:
Journal Volume: 14; Journal Issue: 5; Journal ID: ISSN 1530-6984
Publisher:
American Chemical Society
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE; DFT calculations; Multiferroics; Oxygen vacancies; Polar oxides; Scanning transmission electron microscopy; Transition-metal oxides
OSTI Identifier:
1357051

Mishra, Rohan, Kim, Young-Min, Salafranca, Juan, Kim, Seong Keun, Chang, Seo Hyoung, Bhattacharya, Anand, Fong, Dillon D., Pennycook, Stephen J., Pantelides, Sokrates T., and Borisevich, Albina Y.. Oxygen-Vacancy-Induced Polar Behavior in (LaFeO3)2/(SrFeO3) Superlattices. United States: N. p., Web. doi:10.1021/nl500601d.
Mishra, Rohan, Kim, Young-Min, Salafranca, Juan, Kim, Seong Keun, Chang, Seo Hyoung, Bhattacharya, Anand, Fong, Dillon D., Pennycook, Stephen J., Pantelides, Sokrates T., & Borisevich, Albina Y.. Oxygen-Vacancy-Induced Polar Behavior in (LaFeO3)2/(SrFeO3) Superlattices. United States. doi:10.1021/nl500601d.
Mishra, Rohan, Kim, Young-Min, Salafranca, Juan, Kim, Seong Keun, Chang, Seo Hyoung, Bhattacharya, Anand, Fong, Dillon D., Pennycook, Stephen J., Pantelides, Sokrates T., and Borisevich, Albina Y.. 2014. "Oxygen-Vacancy-Induced Polar Behavior in (LaFeO3)2/(SrFeO3) Superlattices". United States. doi:10.1021/nl500601d. https://www.osti.gov/servlets/purl/1357051.
@article{osti_1357051,
title = {Oxygen-Vacancy-Induced Polar Behavior in (LaFeO3)2/(SrFeO3) Superlattices},
author = {Mishra, Rohan and Kim, Young-Min and Salafranca, Juan and Kim, Seong Keun and Chang, Seo Hyoung and Bhattacharya, Anand and Fong, Dillon D. and Pennycook, Stephen J. and Pantelides, Sokrates T. and Borisevich, Albina Y.},
abstractNote = {Complex oxides displaying ferroelectric and/or multiferroic behavior are of high fundamental and applied interest. In this work, for the first time, we show that it is possible to achieve polar order in a superlattice made up of two nonpolar oxides by means of oxygen vacancy ordering. Using scanning transmission electron microscopy imaging, we show the polar displacement of magnetic Fe ions in a superlattice of (LaFeO3)2/(SrFeO3) grown on a SrTiO3 substrate. Using density functional theory calculations, we systematically study the effect of epitaxial strain, octahedral rotations, and surface terminations in the superlattice and find them to have a negligible effect on the antipolar displacements of the Fe ions lying in between SrO and LaO layers of the superlattice (i.e., within La0.5Sr0.5FeO3 unit cells). The introduction of oxygen vacancies, on the other hand, triggers a polar displacement of the Fe ions. We confirm this important result using electron energy loss spectroscopy, which shows partial oxygen vacancy ordering in the region where polar displacements are observed and an absence of vacancy ordering outside of that area.},
doi = {10.1021/nl500601d},
journal = {Nano Letters},
number = 5,
volume = 14,
place = {United States},
year = {2014},
month = {4}
}