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Title: Interfacial stabilization for epitaxial CuCrO2 delafossites

Abstract

ABO2 delafossites are fascinating materials that exhibit a wide range of physical properties, including giant Rashba spin splitting and anomalous Hall effects, because of their characteristic layered structures composed of noble metal A and strongly correlated BO2 sublayers. However, thin film synthesis is known to be extremely challenging owing to their low symmetry rhombohedral structures, which limit the selection of substrates for thin film epitaxy. Hexagonal lattices, such as those provided by Al2O3(0001) and (111) oriented cubic perovskites, are promising candidates for epitaxy of delafossites. However, the formation of twin domains and impurity phases is hard to suppress, and the nucleation and growth mechanisms thereon have not been studied for the growth of epitaxial delafossites. In this study, we report the epitaxial stabilization of a new interfacial phase formed during pulsed-laser epitaxy of (0001)-oriented CuCrO2 epitaxial thin films on Al2O3 substrates. Through a combined study using scanning transmission electron microscopy/electron-energy loss spectroscopy and density functional theory calculations, we report that the nucleation of a thermodynamically stable, atomically thick CuCr1-xAlxO2 interfacial layer is the critical element for the epitaxy of CuCrO2 delafossites on Al2O3 substrates. This finding provides key insights into the thermodynamic mechanism for the nucleation of intermixing-induced buffer layersmore » that can be used for the growth of other noble-metal-based delafossites, which are known to be challenging due to the difficulty in initial nucleation.« less

Authors:
ORCiD logo [1];  [1]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [2]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES), Materials Sciences and Engineering Division
OSTI Identifier:
1649255
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 10; Journal Issue: 1; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; Surfaces; interfaces; thin films

Citation Formats

Ok, Jong Mok, Yoon, Sangmoon, Lupini, Andrew R., Ganesh, Panchapakesan, Chisholm, Matthew F., and Lee, Ho Nyung. Interfacial stabilization for epitaxial CuCrO2 delafossites. United States: N. p., 2020. Web. doi:10.1038/s41598-020-68275-w.
Ok, Jong Mok, Yoon, Sangmoon, Lupini, Andrew R., Ganesh, Panchapakesan, Chisholm, Matthew F., & Lee, Ho Nyung. Interfacial stabilization for epitaxial CuCrO2 delafossites. United States. https://doi.org/10.1038/s41598-020-68275-w
Ok, Jong Mok, Yoon, Sangmoon, Lupini, Andrew R., Ganesh, Panchapakesan, Chisholm, Matthew F., and Lee, Ho Nyung. Thu . "Interfacial stabilization for epitaxial CuCrO2 delafossites". United States. https://doi.org/10.1038/s41598-020-68275-w. https://www.osti.gov/servlets/purl/1649255.
@article{osti_1649255,
title = {Interfacial stabilization for epitaxial CuCrO2 delafossites},
author = {Ok, Jong Mok and Yoon, Sangmoon and Lupini, Andrew R. and Ganesh, Panchapakesan and Chisholm, Matthew F. and Lee, Ho Nyung},
abstractNote = {ABO2 delafossites are fascinating materials that exhibit a wide range of physical properties, including giant Rashba spin splitting and anomalous Hall effects, because of their characteristic layered structures composed of noble metal A and strongly correlated BO2 sublayers. However, thin film synthesis is known to be extremely challenging owing to their low symmetry rhombohedral structures, which limit the selection of substrates for thin film epitaxy. Hexagonal lattices, such as those provided by Al2O3(0001) and (111) oriented cubic perovskites, are promising candidates for epitaxy of delafossites. However, the formation of twin domains and impurity phases is hard to suppress, and the nucleation and growth mechanisms thereon have not been studied for the growth of epitaxial delafossites. In this study, we report the epitaxial stabilization of a new interfacial phase formed during pulsed-laser epitaxy of (0001)-oriented CuCrO2 epitaxial thin films on Al2O3 substrates. Through a combined study using scanning transmission electron microscopy/electron-energy loss spectroscopy and density functional theory calculations, we report that the nucleation of a thermodynamically stable, atomically thick CuCr1-xAlxO2 interfacial layer is the critical element for the epitaxy of CuCrO2 delafossites on Al2O3 substrates. This finding provides key insights into the thermodynamic mechanism for the nucleation of intermixing-induced buffer layers that can be used for the growth of other noble-metal-based delafossites, which are known to be challenging due to the difficulty in initial nucleation.},
doi = {10.1038/s41598-020-68275-w},
journal = {Scientific Reports},
number = 1,
volume = 10,
place = {United States},
year = {Thu Jul 09 00:00:00 EDT 2020},
month = {Thu Jul 09 00:00:00 EDT 2020}
}

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