Predicting self-diffusion in metal oxides from first principles: The case of oxygen in tetragonal ZrO₂
Author(s)
Yildiz, Bilge; Youssef, Mostafa Youssef Mahmoud
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Theoretical prediction of self-diffusion in a metal oxide in a wide range of thermodynamic conditions has been a long-standing challenge. Here, we establish that combining the formation free energies and migration barriers of all charged oxygen defects as calculated by density functional theory, within the random-walk diffusion theory framework, is a viable approach to predicting oxygen self-diffusion in metal oxides. We demonstrate this approach on tetragonal ZrO2 by calculating oxygen self-diffusivity as a function of temperature and oxygen partial pressure or, alternatively, temperature and off-stoichiometry. Arrhenius analysis on the isobaric (or constant off-stoichiometry) self-diffusivities yields a spectrum of effective activation barriers and prefactors. This provides reconciliation for the wide scatter in the experimentally determined activation barriers and prefactors for many oxides.
Date issued
2014-01Department
Massachusetts Institute of Technology. Department of Nuclear Science and EngineeringJournal
Physical Review B
Publisher
American Physical Society
Citation
Youssef, Mostafa, and Bilge Yildiz. "Predicting self-diffusion in metal oxides from first principles: The case of oxygen in tetragonal ZrO₂." Physical Review B 89 (16 January 2014): 024105. ©2014 American Physical Society.
Version: Final published version
ISSN
1098-0121
1550-235X