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:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Idaho, Moscow, ID (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); National Renewable Energy Lab. (NREL), Golden, CO (United States)
- Lawrence Livermore National Lab. (LLNL), Livermore, CA (United States)
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Univ. of Michigan, Ann Arbor, MI (United States)
- 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 Laboratory (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. doi: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 = {Wed Aug 26 00:00:00 EDT 2015},
month = {Wed Aug 26 00:00:00 EDT 2015}
}
Free Publicly Available Full Text
Publisher's Version of Record
Other availability
Search WorldCat to find libraries that may hold this journal
Cited by: 21 works
Citation information provided by
Web of Science
Web of Science
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.
Works referenced in this record:
Metal-non-metal and other interfaces: the role of image interactions
journal, July 1985
- Stoneham, A. M.; Tasker, P. W.
- Journal of Physics C: Solid State Physics, Vol. 18, Issue 19
Geometrical and Compositional Structure at Metal-Oxide Interfaces: MgO on Fe(001)
journal, July 2001
- Meyerheim, H. L.; Popescu, R.; Kirschner, J.
- Physical Review Letters, Vol. 87, Issue 7
Recent Developments in Irradiation-Resistant Steels
journal, August 2008
- Odette, G. R.; Alinger, M. J.; Wirth, B. D.
- Annual Review of Materials Research, Vol. 38, Issue 1, p. 471-503
Fundamental Influence of C on Adhesion of the Interface
journal, December 2002
- Wang, Xiao-Gang; Smith, John R.; Evans, Anthony
- Physical Review Letters, Vol. 89, Issue 28
Segregation Phenomena at Thermally Grown Al 2 O 3 /Alloy Interfaces
journal, August 2008
- Hou, P. Y.
- Annual Review of Materials Research, Vol. 38, Issue 1
Analysis of Cu segregation to oxide–metal interface of Ni-base alloy by HX-PES
journal, January 2008
- Doi, Takashi; Kitamura, Kazuyuki; Nishiyama, Yoshitaka
- Surface and Interface Analysis, Vol. 40, Issue 3-4
An Atomic Perspective of a Doped Metal-Oxide Interface † , ‡
journal, August 2002
- Jarvis, E. A. A.; Carter, E. A.
- The Journal of Physical Chemistry B, Vol. 106, Issue 33
Massive Interfacial Reconstruction at Misfit Dislocations in Metal/Oxide Interfaces
journal, October 2014
- Choudhury, Samrat; Morgan, Dane; Uberuaga, Blas Pedro
- Scientific Reports, Vol. 4, Issue 1
Nanoscale studies of segregation at coherent heterophase interfaces inα-Fe based systems
journal, May 2004
- Isheim, Dieter; Seidman, David N.
- Surface and Interface Analysis, Vol. 36, Issue 56
Subnanoscale Studies of Segregation at Grain Boundaries: Simulations and Experiments
journal, August 2002
- Seidman, David N.
- Annual Review of Materials Research, Vol. 32, Issue 1
Recycling Metals for the Environment
journal, November 1998
- Wernick, Iddo K.; Themelis, Nickolas J.
- Annual Review of Energy and the Environment, Vol. 23, Issue 1
Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996
- Kresse, G.; Furthmüller, J.
- Physical Review B, Vol. 54, Issue 16, p. 11169-11186
Ab initiomolecular dynamics for liquid metals
journal, January 1993
- Kresse, G.; Hafner, J.
- Physical Review B, Vol. 47, Issue 1, p. 558-561
Influence of sulfur on the adhesion of the nickel/alumina interface
journal, June 2003
- Zhang, W.; Smith, J. R.; Wang, X. -G.
- Physical Review B, Vol. 67, Issue 24
Iron and its dilute substitutional solid solutions
journal, January 1972
- Leslie, W. C.
- Metallurgical and Materials Transactions B, Vol. 3, Issue 1
The formation and evolution of oxide particles in oxide-dispersion-strengthened ferritic steels during processing
journal, April 2013
- Williams, Ceri A.; Unifantowicz, Paulina; Baluc, Nadine
- Acta Materialia, Vol. 61, Issue 6
Nanoscale characterisation of ODS–Eurofer 97 steel: An atom-probe tomography study
journal, May 2010
- Williams, Ceri A.; Marquis, Emmanuelle A.; Cerezo, Alfred
- Journal of Nuclear Materials, Vol. 400, Issue 1
The theory of metal - ceramic interfaces
journal, August 1996
- Finnis, M. W.
- Journal of Physics: Condensed Matter, Vol. 8, Issue 32
Neutron reflection studies of titanium segregation to metal–ceramic interfaces
journal, June 1998
- Derby, Brian; Xiao, Ping; Webster, John
- Physica B: Condensed Matter, Vol. 248, Issue 1-4
Iron Oxidation, Interfacial Expansion, and Buckling at the Interface
journal, March 2006
- Luches, P.; Bellini, V.; Colonna, S.
- Physical Review Letters, Vol. 96, Issue 10
Interface adhesion: effects of plasticity and segregation
journal, November 1999
- Evans, A. G.; Hutchinson, J. W.; Wei, Y.
- Acta Materialia, Vol. 47, Issue 15-16
Adhesion, stability, and bonding at metal/metal-carbide interfaces: Al/WC
journal, February 2002
- Siegel, Donald J.; Hector, Louis G.; Adams, James B.
- Surface Science, Vol. 498, Issue 3
Y 2 O 3 Morphology in an Oxide Dispersion Strengthened FeAl Alloy Prepared by Mechanical Alloying
journal, January 1996
- Inkson, B. J.; Threadgill, P. L.
- MRS Proceedings, Vol. 460
The stability of ionic crystal surfaces
journal, November 1979
- Tasker, P. W.
- Journal of Physics C: Solid State Physics, Vol. 12, Issue 22
Projector augmented-wave method
journal, December 1994
- Blöchl, P. E.
- Physical Review B, Vol. 50, Issue 24, p. 17953-17979
Generalized Gradient Approximation Made Simple
journal, October 1996
- Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
- Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
Quantifying the low-energy limit and spectral resolution in valence electron energy loss spectroscopy
journal, January 2013
- Aguiar, Jeffery A.; Reed, Bryan W.; Ramasse, Quentin M.
- Ultramicroscopy, Vol. 124
Linking Interfacial Step Structure and Chemistry with Locally Enhanced Radiation-Induced Amorphization at Oxide Heterointerfaces
journal, April 2014
- Aguiar, Jeffery A.; Dholabhai, Pratik P.; Bi, Zhenxing
- Advanced Materials Interfaces, Vol. 1, Issue 4
Orientation-specific amorphization and intercalated recrystallization at ion-irradiated SrTiO 3 /MgO interfaces
journal, August 2014
- Aguiar, Jeffery A.; Zhuo, Mujin; Bi, Zhenxing
- Journal of Materials Research, Vol. 29, Issue 16
Mapping strain modulated electronic structure perturbations in mixed phase bismuth ferrite thin films
journal, January 2015
- Krishnan, P. S. Sankara Rama; Aguiar, Jeffery A.; Ramasse, Q. M.
- Journal of Materials Chemistry C, Vol. 3, Issue 8
The formation and evolution of oxide particles in oxide-dispersion-strengthened ferritic steels during processing
journal, April 2013
- Williams, Ceri A.; Unifantowicz, Paulina; Baluc, Nadine
- Acta Materialia, Vol. 61, Issue 6
Quantifying the low-energy limit and spectral resolution in valence electron energy loss spectroscopy
journal, January 2013
- Aguiar, Jeffery A.; Reed, Bryan W.; Ramasse, Quentin M.
- Ultramicroscopy, Vol. 124
Nanometer-scale solute segregation at heterophase interfaces and microstructural evolution of molybdenum nitride precipitates
journal, October 2001
- Isheim, Dieter; Siem, Ellen J.; Seidman, David N.
- Ultramicroscopy, Vol. 89, Issue 1-3
Subnanometer three-dimensional atom-probe investigation of segregation at MgO/Cu ceramic/metal heterophase interfaces
journal, October 2001
- Sebastian, J. T.; Rüsing, J.; Hellman, O. C.
- Ultramicroscopy, Vol. 89, Issue 1-3
The experimental research for production of hydrogen from n-octane through partially oxidizing and steam reforming method
journal, August 2001
- Yanhui, W.
- International Journal of Hydrogen Energy, Vol. 26, Issue 8
Metal–ceramic interfaces studied with high-resolution transmission electron microscopy
journal, November 1999
- de Hosson, J. Th. M.; Groen, H. B.; Kooi, B. J.
- Acta Materialia, Vol. 47, Issue 15-16
Analysis of Gibbsian Segregation at Heterophase Cu-MnO Interfaces
journal, January 2004
- Mogck, Stefan; Kooi, Bart J.; De Hosson, Jeff T.
- Interface Science, Vol. 12, Issue 1
Massive Interfacial Reconstruction at Misfit Dislocations in Metal/Oxide Interfaces
journal, October 2014
- Choudhury, Samrat; Morgan, Dane; Uberuaga, Blas Pedro
- Scientific Reports, Vol. 4, Issue 1
Interfacial mixing of ultrathin Cr films grown on an Fe whisker
journal, January 1996
- Venus, D.; Heinrich, B.
- Physical Review B, Vol. 53, Issue 4
Adhesive energy and charge transfer for MgO/Cu heterophase interfaces
journal, September 1996
- Benedek, R.; Minkoff, M.; Yang, L. H.
- Physical Review B, Vol. 54, Issue 11
First Principles Simulation of a Ceramic Metal Interface with Misfit
journal, April 2000
- Benedek, R.; Alavi, A.; Seidman, D. N.
- Physical Review Letters, Vol. 84, Issue 15
Interface Energy of Semicoherent Metal-Ceramic Interfaces
journal, November 2005
- Johansson, Sven A. E.; Christensen, Mikael; Wahnström, Göran
- Physical Review Letters, Vol. 95, Issue 22
Effect of oxygen vacancies on adhesion at the Nb/Al2O3 and Ni/ZrO2 interfaces
journal, March 2008
- Eremeev, S. V.; Nemirovich-Danchenko, L. Yu.; Kul’kova, S. E.
- Physics of the Solid State, Vol. 50, Issue 3
Works referencing / citing this record:
Beyond Coherent Oxide Heterostructures: Atomic‐Scale Structure of Misfit Dislocations
journal, June 2019
- Dholabhai, Pratik P.; Uberuaga, Blas P.
- Advanced Theory and Simulations, Vol. 2, Issue 9
Semicoherent oxide heterointerfaces: Structure, properties, and implications
journal, October 2019
- Uberuaga, Blas Pedro; Dholabhai, Pratik P.; Pilania, Ghanshyam
- APL Materials, Vol. 7, Issue 10
Segregation and properties at curved vs straight (000) inversion boundaries in piezotronic ZnO bicrystals
journal, December 2019
- Trapp, Maximilian; Keil, Peter; Frömling, Till
- Journal of the American Ceramic Society, Vol. 103, Issue 4