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Title: Interface creation on a mixed-terminated perovskite surface

Abstract

In the field of complex oxide heterostructures, understanding of the initial substrate surface can be critical to fundamental studies regarding the development of emergent properties at the film–substrate interface. For this reason, a considerable amount of effort has gone into the development of techniques to achieve surfaces with single termination for a variety of perovskite single crystals. However, a decisive understanding of how an interface is created when epitaxial growth occurs on a mixed terminated surface remains lacking. Employing in situ synchrotron X-ray scattering during thin film growth by molecular beam epitaxy, we investigate the initial stages of growth on (LaAlO3)(Sr2AlTaO6) (001) substrates with mixed termination. Using LaNiO3 as a model system, we find that the surface layers of the substrate restructure during deposition such that while a NiO2 monolayer is weakly bound, a LaO monolayer bonds strongly, effectively incorporating with (Al, Ta)O2 from the surface and forming a La(Al, Ta)O3 ultrathin film.With regard to the synthesis of high-quality complex oxide heterostructures, it is important that the substrate meet an array of criteria related to the crystal structure, lattice parameter, thermodynamic properties, electrical and optical properties, and so on. In particular, the surface of the substrate should be atomically smooth and exhibit the step-terrace structure ideal for epitaxial thin film growth. Perovskite oxides with the formula ABO3 have two possible (001) surfaces: AO (A-site termination) and BO2 (B-site termination). The ability to consistently achieve one of these surface terminations on SrTiO 3 , i.e., TiO2, has helped SrTiO3 become the predominant oxide in the field.

Authors:
ORCiD logo [1];  [2];  [3]; ORCiD logo [2]; ORCiD logo [4];  [5]; ORCiD logo [5]; ORCiD logo [4]; ORCiD logo [2]
  1. Chinese Academy of Sciences (CAS), Beijing (China); Argonne National Lab. (ANL), Lemont, IL (United States); Univ. of Chinese Academy of Sciences, Beijing (China)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Argonne National Lab. (ANL), Lemont, IL (United States); Chinese Academy of Sciences (CAS), Beijing (China)
  4. Chinese Academy of Sciences (CAS), Beijing (China)
  5. Argonne National Lab. (ANL), Lemont, IL (United States). Advanced Photon Source (APS)
Publication Date:
Research Org.:
Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
Chinese Academy of Sciences (CAS); China Scholarship Council; USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; USDOE
OSTI Identifier:
1765376
Alternate Identifier(s):
OSTI ID: 1765052
Grant/Contract Number:  
AC02-06CH11357; 11U153210485; Y611U21
Resource Type:
Accepted Manuscript
Journal Name:
Applied Physics Letters
Additional Journal Information:
Journal Volume: 118; Journal Issue: 6; Journal ID: ISSN 0003-6951
Publisher:
American Institute of Physics (AIP)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Heterostructures; thin film growth; stoichiometry; x-ray scattering; synchrotrons; epitaxy; perovskites; crystallographic defects; near edge x-ray absorption fine structure spectroscopy; crystallography

Citation Formats

Li, Yan, Wrobel, Friederike, Yan, Xi, Bhattacharya, Anand, Sun, Jirong, Hong, Hawoong, Zhou, Hua, Wang, Huanhua, and Fong, Dillon D. Interface creation on a mixed-terminated perovskite surface. United States: N. p., 2021. Web. doi:10.1063/5.0036279.
Li, Yan, Wrobel, Friederike, Yan, Xi, Bhattacharya, Anand, Sun, Jirong, Hong, Hawoong, Zhou, Hua, Wang, Huanhua, & Fong, Dillon D. Interface creation on a mixed-terminated perovskite surface. United States. https://doi.org/10.1063/5.0036279
Li, Yan, Wrobel, Friederike, Yan, Xi, Bhattacharya, Anand, Sun, Jirong, Hong, Hawoong, Zhou, Hua, Wang, Huanhua, and Fong, Dillon D. Wed . "Interface creation on a mixed-terminated perovskite surface". United States. https://doi.org/10.1063/5.0036279. https://www.osti.gov/servlets/purl/1765376.
@article{osti_1765376,
title = {Interface creation on a mixed-terminated perovskite surface},
author = {Li, Yan and Wrobel, Friederike and Yan, Xi and Bhattacharya, Anand and Sun, Jirong and Hong, Hawoong and Zhou, Hua and Wang, Huanhua and Fong, Dillon D.},
abstractNote = {In the field of complex oxide heterostructures, understanding of the initial substrate surface can be critical to fundamental studies regarding the development of emergent properties at the film–substrate interface. For this reason, a considerable amount of effort has gone into the development of techniques to achieve surfaces with single termination for a variety of perovskite single crystals. However, a decisive understanding of how an interface is created when epitaxial growth occurs on a mixed terminated surface remains lacking. Employing in situ synchrotron X-ray scattering during thin film growth by molecular beam epitaxy, we investigate the initial stages of growth on (LaAlO3)(Sr2AlTaO6) (001) substrates with mixed termination. Using LaNiO3 as a model system, we find that the surface layers of the substrate restructure during deposition such that while a NiO2 monolayer is weakly bound, a LaO monolayer bonds strongly, effectively incorporating with (Al, Ta)O2 from the surface and forming a La(Al, Ta)O3 ultrathin film.With regard to the synthesis of high-quality complex oxide heterostructures, it is important that the substrate meet an array of criteria related to the crystal structure, lattice parameter, thermodynamic properties, electrical and optical properties, and so on. In particular, the surface of the substrate should be atomically smooth and exhibit the step-terrace structure ideal for epitaxial thin film growth. Perovskite oxides with the formula ABO3 have two possible (001) surfaces: AO (A-site termination) and BO2 (B-site termination). The ability to consistently achieve one of these surface terminations on SrTiO 3 , i.e., TiO2, has helped SrTiO3 become the predominant oxide in the field.},
doi = {10.1063/5.0036279},
journal = {Applied Physics Letters},
number = 6,
volume = 118,
place = {United States},
year = {Wed Feb 10 00:00:00 EST 2021},
month = {Wed Feb 10 00:00:00 EST 2021}
}

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