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Title: Three-dimensional atomic scale electron density reconstruction of octahedral tilt epitaxy in functional perovskites

Octahedral tilts are the most ubiquitous distortions in perovskite-related structures that can dramatically influence ferroelectric, magnetic, and electronic properties; yet the paradigm of tilt epitaxy in thin films is barely explored. Non-destructively characterizing such epitaxy in three-dimensions for low symmetry complex tilt systems composed of light anions is a formidable challenge. Here we demonstrate that the interfacial tilt epitaxy can transform ultrathin calcium titanate, a non-polar earth-abundant mineral, into high-temperature polar oxides that last above 900 K. The comprehensive picture of octahedral tilts and polar distortions is revealed by reconstructing the three-dimensional electron density maps across film-substrate interfaces with atomic resolution using coherent Bragg rod analysis. The results are complemented with aberration-corrected transmission electron microscopy,film superstructure reflections, and are in excellent agreement with density functional theory. Conclusively, the study could serve as a broader template for non-destructive, three-dimensional atomic resolution probing of complex low symmetry functional interfaces.
Authors:
 [1] ;  [1] ;  [1] ;  [1] ;  [2] ;  [3] ;  [1] ;  [4] ;  [1]
  1. Pennsylvania State Univ., University Park, PA (United States)
  2. Cornell Univ., Ithaca, NY (United States)
  3. Cornell Univ., Ithaca, NY (United States); Kavli Inst. at Cornell for Nanoscale Science, Ithaca, NY (United States)
  4. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Grant/Contract Number:
AC02-06CH11357
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 9; Journal Issue: 1; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org:
National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE
OSTI Identifier:
1503283

Yuan, Yakun, Lu, Yanfu, Stone, Greg, Wang, Ke, Brooks, Charles M., Schlom, Darrell G., Sinnott, Susan B., Zhou, Hua, and Gopalan, Venkatraman. Three-dimensional atomic scale electron density reconstruction of octahedral tilt epitaxy in functional perovskites. United States: N. p., Web. doi:10.1038/s41467-018-07665-1.
Yuan, Yakun, Lu, Yanfu, Stone, Greg, Wang, Ke, Brooks, Charles M., Schlom, Darrell G., Sinnott, Susan B., Zhou, Hua, & Gopalan, Venkatraman. Three-dimensional atomic scale electron density reconstruction of octahedral tilt epitaxy in functional perovskites. United States. doi:10.1038/s41467-018-07665-1.
Yuan, Yakun, Lu, Yanfu, Stone, Greg, Wang, Ke, Brooks, Charles M., Schlom, Darrell G., Sinnott, Susan B., Zhou, Hua, and Gopalan, Venkatraman. 2018. "Three-dimensional atomic scale electron density reconstruction of octahedral tilt epitaxy in functional perovskites". United States. doi:10.1038/s41467-018-07665-1. https://www.osti.gov/servlets/purl/1503283.
@article{osti_1503283,
title = {Three-dimensional atomic scale electron density reconstruction of octahedral tilt epitaxy in functional perovskites},
author = {Yuan, Yakun and Lu, Yanfu and Stone, Greg and Wang, Ke and Brooks, Charles M. and Schlom, Darrell G. and Sinnott, Susan B. and Zhou, Hua and Gopalan, Venkatraman},
abstractNote = {Octahedral tilts are the most ubiquitous distortions in perovskite-related structures that can dramatically influence ferroelectric, magnetic, and electronic properties; yet the paradigm of tilt epitaxy in thin films is barely explored. Non-destructively characterizing such epitaxy in three-dimensions for low symmetry complex tilt systems composed of light anions is a formidable challenge. Here we demonstrate that the interfacial tilt epitaxy can transform ultrathin calcium titanate, a non-polar earth-abundant mineral, into high-temperature polar oxides that last above 900 K. The comprehensive picture of octahedral tilts and polar distortions is revealed by reconstructing the three-dimensional electron density maps across film-substrate interfaces with atomic resolution using coherent Bragg rod analysis. The results are complemented with aberration-corrected transmission electron microscopy,film superstructure reflections, and are in excellent agreement with density functional theory. Conclusively, the study could serve as a broader template for non-destructive, three-dimensional atomic resolution probing of complex low symmetry functional interfaces.},
doi = {10.1038/s41467-018-07665-1},
journal = {Nature Communications},
number = 1,
volume = 9,
place = {United States},
year = {2018},
month = {12}
}

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