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Title: Non-uniform solute segregation at semi-coherent metal/oxide interfaces

Abstract

The properties and performance of metal/oxide nanocomposites are governed by the structure and chemistry of the metal/oxide interfaces. Here we report an integrated theoretical and experimental study examining the role of interfacial structure, particularly misfit dislocations, on solute segregation at a metal/oxide interface. We find that the local oxygen environment, which varies significantly between the misfit dislocations and the coherent terraces, dictates the segregation tendency of solutes to the interface. Depending on the nature of the solute and local oxygen content, segregation to misfit dislocations can change from attraction to repulsion, revealing the complex interplay between chemistry and structure at metal/oxide interfaces. These findings indicate that the solute chemistry at misfit dislocations is controlled by the dislocation density and oxygen content. As a result, fundamental thermodynamic concepts – the Hume-Rothery rules and the Ellingham diagram – qualitatively predict the segregation behavior of solutes to such interfaces, providing design rules for novel interfacial chemistries.

Authors:
 [1];  [2];  [3];  [3];  [4];  [5]
  1. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Idaho, Moscow, ID (United States)
  2. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
  3. Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
  4. Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Michigan, Ann Arbor, MI (United States)
  5. Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Publication Date:
Research Org.:
Energy Frontier Research Centers (EFRC) (United States). Center for Materials at Irradiation and Mechanical Extremes (CMIME); Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1236769
Report Number(s):
LA-UR-15-25964
Journal ID: ISSN 2045-2322; srep13086
Grant/Contract Number:  
AC52-06NA25396
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 5; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; composites; electronic structure; surfaces, interfaces and thin films

Citation Formats

Choudhury, Samrat, Aguiar, Jeffery A., Fluss, Michael J., Hsiung, Luke L., Misra, Amit, and Uberuaga, Blas P.. Non-uniform solute segregation at semi-coherent metal/oxide interfaces. United States: N. p., 2015. Web. https://doi.org/10.1038/srep13086.
Choudhury, Samrat, Aguiar, Jeffery A., Fluss, Michael J., Hsiung, Luke L., Misra, Amit, & Uberuaga, Blas P.. Non-uniform solute segregation at semi-coherent metal/oxide interfaces. United States. https://doi.org/10.1038/srep13086
Choudhury, Samrat, Aguiar, Jeffery A., Fluss, Michael J., Hsiung, Luke L., Misra, Amit, and Uberuaga, Blas P.. Wed . "Non-uniform solute segregation at semi-coherent metal/oxide interfaces". United States. https://doi.org/10.1038/srep13086. https://www.osti.gov/servlets/purl/1236769.
@article{osti_1236769,
title = {Non-uniform solute segregation at semi-coherent metal/oxide interfaces},
author = {Choudhury, Samrat and Aguiar, Jeffery A. and Fluss, Michael J. and Hsiung, Luke L. and Misra, Amit and Uberuaga, Blas P.},
abstractNote = {The properties and performance of metal/oxide nanocomposites are governed by the structure and chemistry of the metal/oxide interfaces. Here we report an integrated theoretical and experimental study examining the role of interfacial structure, particularly misfit dislocations, on solute segregation at a metal/oxide interface. We find that the local oxygen environment, which varies significantly between the misfit dislocations and the coherent terraces, dictates the segregation tendency of solutes to the interface. Depending on the nature of the solute and local oxygen content, segregation to misfit dislocations can change from attraction to repulsion, revealing the complex interplay between chemistry and structure at metal/oxide interfaces. These findings indicate that the solute chemistry at misfit dislocations is controlled by the dislocation density and oxygen content. As a result, fundamental thermodynamic concepts – the Hume-Rothery rules and the Ellingham diagram – qualitatively predict the segregation behavior of solutes to such interfaces, providing design rules for novel interfacial chemistries.},
doi = {10.1038/srep13086},
journal = {Scientific Reports},
number = ,
volume = 5,
place = {United States},
year = {2015},
month = {8}
}

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Cited by: 5 works
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    Works referencing / citing this record:

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