The effects of cation–anion clustering on defect migration in MgAl2O4
Abstract
Magnesium aluminate spinel (MgAl2O4), like many other ceramic materials, offers a range of technological applications, from nuclear reactor materials to military body armor. For many of these applications, it is critical to understand both the formation and evolution of lattice defects throughout the lifetime of the material. We use the Speculatively Parallel Temperature Accelerated Dynamics (SpecTAD) method to investigate the effects of di-vacancy and di-interstitial formation on the mobility of the component defects. From long-time trajectories of the state-to-state dynamics, we characterize the migration pathways of defect clusters, and calculate their self-diffusion constants across a range of temperatures. We find that the clustering of Al and O vacancies drastically reduces the mobility of both defects, while the clustering of Mg and O vacancies completely immobilizes them. For interstitials, we find that the clustering of Mg and O defects greatly reduces O interstitial mobility, but has only a weak effect on Mg. Lastly, these findings illuminate important new details regarding defect kinetics relevant to the application of MgAl2O4 in extreme environments.
- Authors:
-
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Publication Date:
- Research Org.:
- Los Alamos National Lab. (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1329597
- Report Number(s):
- LA-UR-16-23859
Journal ID: ISSN 1463-9076; PPCPFQ
- Grant/Contract Number:
- AC52-06NA25396
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Physical Chemistry Chemical Physics. PCCP
- Additional Journal Information:
- Journal Volume: 18; Journal Issue: 29; Journal ID: ISSN 1463-9076
- Publisher:
- Royal Society of Chemistry
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; material science
Citation Formats
Zamora, Richard J., Voter, Arthur F., Perez, Danny, Perriot, Romain, and Uberuaga, Blas P. The effects of cation–anion clustering on defect migration in MgAl2O4. United States: N. p., 2016.
Web. doi:10.1039/C6CP03931F.
Zamora, Richard J., Voter, Arthur F., Perez, Danny, Perriot, Romain, & Uberuaga, Blas P. The effects of cation–anion clustering on defect migration in MgAl2O4. United States. https://doi.org/10.1039/C6CP03931F
Zamora, Richard J., Voter, Arthur F., Perez, Danny, Perriot, Romain, and Uberuaga, Blas P. Tue .
"The effects of cation–anion clustering on defect migration in MgAl2O4". United States. https://doi.org/10.1039/C6CP03931F. https://www.osti.gov/servlets/purl/1329597.
@article{osti_1329597,
title = {The effects of cation–anion clustering on defect migration in MgAl2O4},
author = {Zamora, Richard J. and Voter, Arthur F. and Perez, Danny and Perriot, Romain and Uberuaga, Blas P.},
abstractNote = {Magnesium aluminate spinel (MgAl2O4), like many other ceramic materials, offers a range of technological applications, from nuclear reactor materials to military body armor. For many of these applications, it is critical to understand both the formation and evolution of lattice defects throughout the lifetime of the material. We use the Speculatively Parallel Temperature Accelerated Dynamics (SpecTAD) method to investigate the effects of di-vacancy and di-interstitial formation on the mobility of the component defects. From long-time trajectories of the state-to-state dynamics, we characterize the migration pathways of defect clusters, and calculate their self-diffusion constants across a range of temperatures. We find that the clustering of Al and O vacancies drastically reduces the mobility of both defects, while the clustering of Mg and O vacancies completely immobilizes them. For interstitials, we find that the clustering of Mg and O defects greatly reduces O interstitial mobility, but has only a weak effect on Mg. Lastly, these findings illuminate important new details regarding defect kinetics relevant to the application of MgAl2O4 in extreme environments.},
doi = {10.1039/C6CP03931F},
journal = {Physical Chemistry Chemical Physics. PCCP},
number = 29,
volume = 18,
place = {United States},
year = {Tue Jun 28 00:00:00 EDT 2016},
month = {Tue Jun 28 00:00:00 EDT 2016}
}
Web of Science
Works referenced in this record:
Temperature-accelerated dynamics for simulation of infrequent events
journal, June 2000
- So/rensen, Mads R.; Voter, Arthur F.
- The Journal of Chemical Physics, Vol. 112, Issue 21
Interpreting oxygen vacancy migration mechanisms in oxides using the layered structure motif
journal, June 2015
- Uberuaga, Blas Pedro; Sickafus, Kurt E.
- Computational Materials Science, Vol. 103
Structure of Spinel
journal, December 1999
- Sickafus, Kurt E.; Wills, John M.; Grimes, Norman W.
- Journal of the American Ceramic Society, Vol. 82, Issue 12
Exploiting past visits or minimum-barrier knowledge to gain further boost in the temperature-accelerated dynamics method
journal, January 2002
- Montalenti, F.; Voter, A. F.
- The Journal of Chemical Physics, Vol. 116, Issue 12
The Modern Temperature-Accelerated Dynamics Approach
journal, June 2016
- Zamora, Richard J.; Uberuaga, Blas P.; Perez, Danny
- Annual Review of Chemical and Biomolecular Engineering, Vol. 7, Issue 1
Low- and high-temperature spinel (MgAl 2 O 4 ): studies on natural single crystals by neutron diffraction
journal, August 1981
- Baumgartner, O.; Preisinger, A.; Heger, G.
- Acta Crystallographica Section A Foundations of Crystallography, Vol. 37, Issue a1
Defect processes in MgAl2O4 spinel
journal, June 2008
- Ball, J. A.; Murphy, S. T.; Grimes, R. W.
- Solid State Sciences, Vol. 10, Issue 6
A climbing image nudged elastic band method for finding saddle points and minimum energy paths
journal, December 2000
- Henkelman, Graeme; Uberuaga, Blas P.; Jónsson, Hannes
- The Journal of Chemical Physics, Vol. 113, Issue 22, p. 9901-9904
Interstitial and vacancy mediated transport mechanisms in perovskites: A comparison of chemistry and potentials
journal, December 2013
- Uberuaga, Blas Pedro; Vernon, Louis J.
- Solid State Ionics, Vol. 253
Frequency factors and isotope effects in solid state rate processes
journal, January 1957
- Vineyard, George H.
- Journal of Physics and Chemistry of Solids, Vol. 3, Issue 1-2
Cation diffusion in magnesium aluminate spinel
journal, February 2009
- Murphy, S. T.; Uberuaga, B. P.; Ball, J. B.
- Solid State Ionics, Vol. 180, Issue 1
Atomistic simulations of radiation-induced defect formation in spinels: , , and
journal, December 2006
- Bacorisen, D.; Smith, Roger; Uberuaga, B. P.
- Physical Review B, Vol. 74, Issue 21
An extended hardness limit in bulk nanoceramics
journal, May 2014
- Wollmershauser, James A.; Feigelson, Boris N.; Gorzkowski, Edward P.
- Acta Materialia, Vol. 69
Heavy ion induced damage in MgAl2O4, an inert matrix candidate for the transmutation of minor actinides
journal, June 1999
- Wiss, T.; Matzke, Hj.
- Radiation Measurements, Vol. 31, Issue 1-6
Defect Reactions and the Controlling Mechanism in the Sintering of Magnesium Aluminate Spinel
journal, April 1999
- Ting, Ching-Jui; Lu, Hong-Yang
- Journal of the American Ceramic Society, Vol. 82, Issue 4
Materials research on inert matrices: a screening study
journal, August 1999
- Matzke, Hj; Rondinella, V. V.; Wiss, T.
- Journal of Nuclear Materials, Vol. 274, Issue 1-2
Defect kinetics in spinels: Long-time simulations of , , and
journal, March 2007
- Uberuaga, B. P.; Bacorisen, D.; Smith, Roger
- Physical Review B, Vol. 75, Issue 10
Insights into dynamic processes of cations in pyrochlores and other complex oxides
journal, January 2015
- Uberuaga, Blas Pedro; Perriot, Romain
- Physical Chemistry Chemical Physics, Vol. 17, Issue 37
Cation disorder in Mg O ( = Al, Ga, In) spinels from first principles
journal, July 2012
- Jiang, Chao; Sickafus, Kurt E.; Stanek, Christopher R.
- Physical Review B, Vol. 86, Issue 2
Works referencing / citing this record:
Speculation and replication in temperature accelerated dynamics
journal, February 2018
- Zamora, Richard J.; Perez, Danny; Voter, Arthur F.
- Journal of Materials Research, Vol. 33, Issue 7