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 language | English |
|---|---|
| Article number | 224105 |
| Journal | Physical Review B - Condensed Matter and Materials Physics |
| Volume | 83 |
| Issue number | 22 |
| DOIs | |
| Publication status | Published - 2011 Jun 21 |
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All Science Journal Classification (ASJC) codes
- Electronic, Optical and Magnetic Materials
- Condensed Matter Physics
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Free energy of defect formation : Thermodynamics of anion Frenkel pairs in indium oxide. / Walsh, Aron; Sokol, Alexey A.; Catlow, C. Richard A.
In: Physical Review B - Condensed Matter and Materials Physics, Vol. 83, No. 22, 224105, 21.06.2011.Research output: Contribution to journal › Article
TY - JOUR
T1 - Free energy of defect formation
T2 - Thermodynamics of anion Frenkel pairs in indium oxide
AU - Walsh, Aron
AU - Sokol, Alexey A.
AU - Catlow, C. Richard A.
PY - 2011/6/21
Y1 - 2011/6/21
N2 - 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.
AB - 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.
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U2 - 10.1103/PhysRevB.83.224105
DO - 10.1103/PhysRevB.83.224105
M3 - Article
AN - SCOPUS:79961135485
VL - 83
JO - Physical Review B-Condensed Matter
JF - Physical Review B-Condensed Matter
SN - 1098-0121
IS - 22
M1 - 224105
ER -