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Title: Unexpected crystalline homogeneity from the disordered bond network in La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films

Abstract

Designing and understanding functional electronic and magnetic properties in perovskite oxides requires controlling and tuning the underlying crystal lattice. In this work, we report the structure, including oxygen and cation positions, of a single-crystal, entropy stabilized perovskite oxide film of La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 grown on SrTiO3 (001). The parent materials range from orthorhombic (LaCrO3, LaMnO3, and LaFeO3) to rhombohedral (LaCoO3 and LaNiO3), and first principles calculations indicate that these structural motifs are nearly degenerate in energy and should be highly distorted site to site. Despite this extraordinary local configurational disorder on the B-site sublattice, we find a structure with unexpected macroscopic crystalline homogeneity with a clear orthorhombic unit cell, whose orientation is demonstrated to be controlled by the strain and crystal structure of the substrate for films grown on (La0.3Sr0.7)(Al0.65Ta0.35)O3 and NdGaO3 (110). Furthermore, quantification of the atom positions within the unit cell reveals that the orthorhombic distortions are small, close to LaCrO3, which may be driven by a combination of disorder averaging and the average ionic radii. This is a step toward understanding the rules for designing crystal motifs and tuning functional properties through controlled configurational complexity.

Authors:
 [1]; ORCiD logo [1];  [1]; ORCiD logo [1];  [1];  [1]; ORCiD logo [1]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division
OSTI Identifier:
1651333
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 4; Journal Issue: 5; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
Complex oxides; perovskite; transition-metal oxides; epitaxy; configurationally complex materials; crystal structure; entropy stabilized oxides; oxygen octahedra

Citation Formats

Brahlek, Matthew, Mazza, Alessandro R., Pitike, Krishna Chaitanya, Skoropata, Elizabeth, Lapano, Jason, Eres, Gyula, Cooper, Valentino R., and Ward, T. Zac. Unexpected crystalline homogeneity from the disordered bond network in La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films. United States: N. p., 2020. Web. doi:10.1103/physrevmaterials.4.054407.
Brahlek, Matthew, Mazza, Alessandro R., Pitike, Krishna Chaitanya, Skoropata, Elizabeth, Lapano, Jason, Eres, Gyula, Cooper, Valentino R., & Ward, T. Zac. Unexpected crystalline homogeneity from the disordered bond network in La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films. United States. doi:10.1103/physrevmaterials.4.054407.
Brahlek, Matthew, Mazza, Alessandro R., Pitike, Krishna Chaitanya, Skoropata, Elizabeth, Lapano, Jason, Eres, Gyula, Cooper, Valentino R., and Ward, T. Zac. Tue . "Unexpected crystalline homogeneity from the disordered bond network in La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films". United States. doi:10.1103/physrevmaterials.4.054407.
@article{osti_1651333,
title = {Unexpected crystalline homogeneity from the disordered bond network in La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 films},
author = {Brahlek, Matthew and Mazza, Alessandro R. and Pitike, Krishna Chaitanya and Skoropata, Elizabeth and Lapano, Jason and Eres, Gyula and Cooper, Valentino R. and Ward, T. Zac},
abstractNote = {Designing and understanding functional electronic and magnetic properties in perovskite oxides requires controlling and tuning the underlying crystal lattice. In this work, we report the structure, including oxygen and cation positions, of a single-crystal, entropy stabilized perovskite oxide film of La(Cr0.2Mn0.2Fe0.2Co0.2Ni0.2)O3 grown on SrTiO3 (001). The parent materials range from orthorhombic (LaCrO3, LaMnO3, and LaFeO3) to rhombohedral (LaCoO3 and LaNiO3), and first principles calculations indicate that these structural motifs are nearly degenerate in energy and should be highly distorted site to site. Despite this extraordinary local configurational disorder on the B-site sublattice, we find a structure with unexpected macroscopic crystalline homogeneity with a clear orthorhombic unit cell, whose orientation is demonstrated to be controlled by the strain and crystal structure of the substrate for films grown on (La0.3Sr0.7)(Al0.65Ta0.35)O3 and NdGaO3 (110). Furthermore, quantification of the atom positions within the unit cell reveals that the orthorhombic distortions are small, close to LaCrO3, which may be driven by a combination of disorder averaging and the average ionic radii. This is a step toward understanding the rules for designing crystal motifs and tuning functional properties through controlled configurational complexity.},
doi = {10.1103/physrevmaterials.4.054407},
journal = {Physical Review Materials},
number = 5,
volume = 4,
place = {United States},
year = {2020},
month = {5}
}

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