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Title: Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide

Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden-Popper (RP), A n+1 B n O 3n+1 , thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Sr n+1 Ti n O 3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases. We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure.
Authors:
 [1] ;  [2] ;  [3] ;  [2] ;  [4] ;  [5] ; ORCiD logo [6] ;  [7] ;  [1] ;  [1]
  1. Pennsylvania State Univ., University Park, PA (United States). Dept. of Material Sciences and Engineering
  2. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). Molecular Foundry
  3. Univ. of Minnesota, Minneapolis, MN (United States)
  4. Pennsylvania State Univ., University Park, PA (United States). Dept. of Material Sciences and Engineering; Cornell Univ., Ithaca, NY (United States). Dept. of Materials Science and Engineering
  5. Pennsylvania State Univ., University Park, PA (United States)
  6. Cornell Univ., Ithaca, NY (United States)
  7. Cornell Univ., Ithaca, NY (United States). Dept. of Materials Science and Engineering
Publication Date:
Grant/Contract Number:
AC02-05CH11231; DMR-1420620; DMR-1210588; DMR-1056441
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 7; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (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; ferroelectrics and multiferroics; transmission electron microscopy
OSTI Identifier:
1377432

Stone, Greg, Ophus, Colin, Birol, Turan, Ciston, Jim, Lee, Che-Hui, Wang, Ke, Fennie, Craig J., Schlom, Darrell G., Alem, Nasim, and Gopalan, Venkatraman. Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide. United States: N. p., Web. doi:10.1038/ncomms12572.
Stone, Greg, Ophus, Colin, Birol, Turan, Ciston, Jim, Lee, Che-Hui, Wang, Ke, Fennie, Craig J., Schlom, Darrell G., Alem, Nasim, & Gopalan, Venkatraman. Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide. United States. doi:10.1038/ncomms12572.
Stone, Greg, Ophus, Colin, Birol, Turan, Ciston, Jim, Lee, Che-Hui, Wang, Ke, Fennie, Craig J., Schlom, Darrell G., Alem, Nasim, and Gopalan, Venkatraman. 2016. "Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide". United States. doi:10.1038/ncomms12572. https://www.osti.gov/servlets/purl/1377432.
@article{osti_1377432,
title = {Atomic scale imaging of competing polar states in a Ruddlesden–Popper layered oxide},
author = {Stone, Greg and Ophus, Colin and Birol, Turan and Ciston, Jim and Lee, Che-Hui and Wang, Ke and Fennie, Craig J. and Schlom, Darrell G. and Alem, Nasim and Gopalan, Venkatraman},
abstractNote = {Layered complex oxides offer an unusually rich materials platform for emergent phenomena through many built-in design knobs such as varied topologies, chemical ordering schemes and geometric tuning of the structure. A multitude of polar phases are predicted to compete in Ruddlesden-Popper (RP), A n+1 B n O 3n+1 , thin films by tuning layer dimension (n) and strain; however, direct atomic-scale evidence for such competing states is currently absent. Using aberration-corrected scanning transmission electron microscopy with sub-Ångstrom resolution in Sr n+1 Ti n O 3n+1 thin films, we demonstrate the coexistence of antiferroelectric, ferroelectric and new ordered and low-symmetry phases. We also directly image the atomic rumpling of the rock salt layer, a critical feature in RP structures that is responsible for the competing phases; exceptional quantitative agreement between electron microscopy and density functional theory is demonstrated. The study shows that layered topologies can enable multifunctionality through highly competitive phases exhibiting diverse phenomena in a single structure.},
doi = {10.1038/ncomms12572},
journal = {Nature Communications},
number = ,
volume = 7,
place = {United States},
year = {2016},
month = {8}
}

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