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Title: Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate

Abstract

In this study, we address the fundamental issue of growth of perovskite ultra-thin films under the condition of a strong polar mismatch at the heterointerface exemplified by the growth of a correlated metal LaNiO3 on the band insulator SrTiO3 along the pseudo cubic [111] direction. While in general the metallic LaNiO3 film can effectively screen this polarity mismatch, we establish that in the ultra-thin limit, films are insulating in nature and require additional chemical and structural reconstruction to compensate for such mismatch. A combination of in-situ reflection high-energy electron diffraction recorded during the growth, X-ray diffraction, and synchrotron based resonant X-ray spectroscopy reveal the formation of a chemical phase La2Ni2O5 (Ni2+) for a few unit-cell thick films. First-principles layer-resolved calculations of the potential energy across the nominal LaNiO3/SrTiO3 interface confirm that the oxygen vacancies can efficiently reduce the electric field at the interface.

Authors:
 [1];  [1];  [1];  [1];  [1];  [1];  [2];  [1];  [1]
  1. University of Arkansas, Fayetteville, AR (United States). Dept. of Physics.
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1221158
Alternate Identifier(s):
OSTI ID: 1241336
Grant/Contract Number:  
AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 4; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; electronic properties and materials; surfaces; interfaces and thin films; surfaces, interfaces and thin films

Citation Formats

Middey, S., Rivero, P., Meyers, D., Kareev, M., Liu, X., Cao, Y., Freeland, J. W., Barraza-Lopez, S., and Chakhalian, J. Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate. United States: N. p., 2014. Web. doi:10.1038/srep06819.
Middey, S., Rivero, P., Meyers, D., Kareev, M., Liu, X., Cao, Y., Freeland, J. W., Barraza-Lopez, S., & Chakhalian, J. Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate. United States. https://doi.org/10.1038/srep06819
Middey, S., Rivero, P., Meyers, D., Kareev, M., Liu, X., Cao, Y., Freeland, J. W., Barraza-Lopez, S., and Chakhalian, J. Wed . "Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate". United States. https://doi.org/10.1038/srep06819. https://www.osti.gov/servlets/purl/1221158.
@article{osti_1221158,
title = {Polarity compensation in ultra-thin films of complex oxides: The case of a perovskite nickelate},
author = {Middey, S. and Rivero, P. and Meyers, D. and Kareev, M. and Liu, X. and Cao, Y. and Freeland, J. W. and Barraza-Lopez, S. and Chakhalian, J.},
abstractNote = {In this study, we address the fundamental issue of growth of perovskite ultra-thin films under the condition of a strong polar mismatch at the heterointerface exemplified by the growth of a correlated metal LaNiO3 on the band insulator SrTiO3 along the pseudo cubic [111] direction. While in general the metallic LaNiO3 film can effectively screen this polarity mismatch, we establish that in the ultra-thin limit, films are insulating in nature and require additional chemical and structural reconstruction to compensate for such mismatch. A combination of in-situ reflection high-energy electron diffraction recorded during the growth, X-ray diffraction, and synchrotron based resonant X-ray spectroscopy reveal the formation of a chemical phase La2Ni2O5 (Ni2+) for a few unit-cell thick films. First-principles layer-resolved calculations of the potential energy across the nominal LaNiO3/SrTiO3 interface confirm that the oxygen vacancies can efficiently reduce the electric field at the interface.},
doi = {10.1038/srep06819},
journal = {Scientific Reports},
number = ,
volume = 4,
place = {United States},
year = {Wed Oct 29 00:00:00 EDT 2014},
month = {Wed Oct 29 00:00:00 EDT 2014}
}

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