Free energy of defect formation: Thermodynamics of anion Frenkel pairs in indium oxide

Aron Walsh, A A Sokol, C R A Catlow

Research output: Contribution to journalArticle

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Abstract

The temperature-dependent free energies, entropies, and enthalpies for the formation of anion Frenkel pairs in In2O3 are reported, as calculated within the Mott-Littleton embedded-cluster approach, by exploiting the relationship between isobaric and isochoric thermodynamic processes. Our model for In2O3 proves particularly successful in the reproduction and prediction of the thermoelastic properties, including heat capacity, compressibility, and thermal expansion in the high-temperature regime. We employ this model to predict the thermal behavior of oxygen vacancy and oxygen interstitial defects. Aggregation of the point defects is energetically favorable and dampens the temperature dependence of defect formation, with a decreased free volume of defect formation. The results highlight the contribution of point defects to the high-temperature thermal expansion of indium sesquioxide, as well as the appreciable temperature dependence of the thermodynamic potentials, including enthalpy and free energy, associated with defect formation in general. A transferable procedure for calculating such thermodynamic parameters is presented.
Original languageEnglish
Article number224105
JournalPhysical Review B
Volume83
Issue number22
DOIs
Publication statusPublished - 2011

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indium oxides
Indium
Free energy
Anions
Negative ions
free energy
Thermodynamics
anions
thermodynamics
Defects
Oxides
defects
point defects
thermal expansion
Point defects
enthalpy
Thermal expansion
Enthalpy
Temperature
temperature dependence

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Free energy of defect formation: Thermodynamics of anion Frenkel pairs in indium oxide. / Walsh, Aron; Sokol, A A; Catlow, C R A.

In: Physical Review B, Vol. 83, No. 22, 224105, 2011.

Research output: Contribution to journalArticle

Walsh, Aron ; Sokol, A A ; Catlow, C R A. / Free energy of defect formation: Thermodynamics of anion Frenkel pairs in indium oxide. In: Physical Review B. 2011 ; Vol. 83, No. 22.
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