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

Yuan, Yakun; Lu, Yanfu; Stone, Greg; Wang, Ke; Brooks, Charles M.; Schlom, Darrell G.; Sinnott, Susan B.; Zhou, Hua; Gopalan, Venkatraman

doi:10.1038/s41467-018-07665-1

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

Journal Article · 06 December 2018 · Nature Communications

DOI: https://doi.org/10.1038/s41467-018-07665-1 · OSTI ID:1503283

Yuan, Yakun ^[1]; Lu, Yanfu ^[1]; Stone, Greg ^[1]; Wang, Ke ^[1]; Brooks, Charles M. ^[2]; Schlom, Darrell G. ^[3]; Sinnott, Susan B. ^[1]; Zhou, Hua ^[4]; Gopalan, Venkatraman ^[1]

Pennsylvania State Univ., University Park, PA (United States)
Cornell Univ., Ithaca, NY (United States)
Cornell Univ., Ithaca, NY (United States); Kavli Inst. at Cornell for Nanoscale Science, Ithaca, NY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

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.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF); USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1503283

Journal Information:: Nature Communications, Journal Name: Nature Communications Journal Issue: 1 Vol. 9; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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