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Title: Self-healing Growth of LaNiO3 on a Mixed-Terminated Perovskite Surface

Abstract

Developing atomic-scale synthesis control is a prerequisite for understanding and engineering the exotic physics inherent to transition-metal oxide heterostructures. Thus, far, however, the number of materials systems explored has been extremely limited, particularly with regard to the crystalline substrate, which is routinely SrTiO3. Here, we investigate the growth of a rare-earth nickelate-LaNiO3-on (LaAlO3)(Sr2AlTaO6) (LSAT) (001) by oxide molecular beam epitaxy (MBE). Whereas the LSAT substrates are smooth, they do not exhibit the single surface termination usually assumed necessary for control over the interface structure. Performing both nonresonant and resonant anomalous in situ synchrotron surface X-ray scattering during MBE growth, we show that reproducible heterostructures can be achieved regardless of both the mixed surface termination and the layer-by-layer deposition sequence. The rearrangement of the layers occurs dynamically during growth, resulting in the fabrication of high-quality LaNiO3/LSAT heterostructures with a sharp and consistent interfacial structure. This is due to the thermodynamics of the deposition window as well as the nature of the chemical species at interfaces-here, the flexible charge state of nickel at the oxide surface. This has important implications regarding the use of a wider variety of substrates for fundamental studies on complex oxide synthesis.

Authors:
ORCiD logo [1];  [2]; ORCiD logo [3]; ORCiD logo [2];  [2];  [4]; ORCiD logo [2];  [5]; ORCiD logo [2]; ORCiD logo [4]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]
  1. Chinese Academy of Sciences (CAS), Beijing (China); Argonne National Lab. (ANL), Lemont, IL (United States); University of Chinese Academy of Sciences, Beijing (China)
  2. Argonne National Lab. (ANL), Lemont, IL (United States)
  3. Jilin Univ., Changchun (China)
  4. Chinese Academy of Sciences (CAS), Beijing (China); University of Chinese Academy of Sciences, Beijing (China)
  5. Chinese Academy of Sciences (CAS), Beijing (China)
Publication Date:
Research Org.:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; Chinese Academy of Sciences (CAS); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities Division; National Natural Science Foundation of China (NSFC)
OSTI Identifier:
1874046
Grant/Contract Number:  
AC02-06CH11357; 113111KYSB20190052; U1532104; 11934016; 11921004
Resource Type:
Accepted Manuscript
Journal Name:
ACS Applied Materials and Interfaces
Additional Journal Information:
Journal Volume: 14; Journal Issue: 14; Journal ID: ISSN 1944-8244
Publisher:
American Chemical Society (ACS)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; LaNiO3; in situ surface x-ray scattering; molecular beam epitaxy; mixed surface termination; layer-by-layer deposition sequence; dynamic rearrangement

Citation Formats

Li, Yan, Wrobel, Friederike, Cheng, Yingjie, Yan, Xi, Cao, Hui, Zhang, Zhongying, Bhattacharya, Anand, Sun, Jirong, Hong, Hawoong, Wang, Huanhua, Liu, Yuzi, Zhou, Hua, and Fong, Dillon D. Self-healing Growth of LaNiO3 on a Mixed-Terminated Perovskite Surface. United States: N. p., 2022. Web. doi:10.1021/acsami.2c02357.
Li, Yan, Wrobel, Friederike, Cheng, Yingjie, Yan, Xi, Cao, Hui, Zhang, Zhongying, Bhattacharya, Anand, Sun, Jirong, Hong, Hawoong, Wang, Huanhua, Liu, Yuzi, Zhou, Hua, & Fong, Dillon D. Self-healing Growth of LaNiO3 on a Mixed-Terminated Perovskite Surface. United States. https://doi.org/10.1021/acsami.2c02357
Li, Yan, Wrobel, Friederike, Cheng, Yingjie, Yan, Xi, Cao, Hui, Zhang, Zhongying, Bhattacharya, Anand, Sun, Jirong, Hong, Hawoong, Wang, Huanhua, Liu, Yuzi, Zhou, Hua, and Fong, Dillon D. Wed . "Self-healing Growth of LaNiO3 on a Mixed-Terminated Perovskite Surface". United States. https://doi.org/10.1021/acsami.2c02357. https://www.osti.gov/servlets/purl/1874046.
@article{osti_1874046,
title = {Self-healing Growth of LaNiO3 on a Mixed-Terminated Perovskite Surface},
author = {Li, Yan and Wrobel, Friederike and Cheng, Yingjie and Yan, Xi and Cao, Hui and Zhang, Zhongying and Bhattacharya, Anand and Sun, Jirong and Hong, Hawoong and Wang, Huanhua and Liu, Yuzi and Zhou, Hua and Fong, Dillon D.},
abstractNote = {Developing atomic-scale synthesis control is a prerequisite for understanding and engineering the exotic physics inherent to transition-metal oxide heterostructures. Thus, far, however, the number of materials systems explored has been extremely limited, particularly with regard to the crystalline substrate, which is routinely SrTiO3. Here, we investigate the growth of a rare-earth nickelate-LaNiO3-on (LaAlO3)(Sr2AlTaO6) (LSAT) (001) by oxide molecular beam epitaxy (MBE). Whereas the LSAT substrates are smooth, they do not exhibit the single surface termination usually assumed necessary for control over the interface structure. Performing both nonresonant and resonant anomalous in situ synchrotron surface X-ray scattering during MBE growth, we show that reproducible heterostructures can be achieved regardless of both the mixed surface termination and the layer-by-layer deposition sequence. The rearrangement of the layers occurs dynamically during growth, resulting in the fabrication of high-quality LaNiO3/LSAT heterostructures with a sharp and consistent interfacial structure. This is due to the thermodynamics of the deposition window as well as the nature of the chemical species at interfaces-here, the flexible charge state of nickel at the oxide surface. This has important implications regarding the use of a wider variety of substrates for fundamental studies on complex oxide synthesis.},
doi = {10.1021/acsami.2c02357},
journal = {ACS Applied Materials and Interfaces},
number = 14,
volume = 14,
place = {United States},
year = {Wed Mar 30 00:00:00 EDT 2022},
month = {Wed Mar 30 00:00:00 EDT 2022}
}

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