Thermal conductivity of ThO2: Effect of point defect disorder.

Thoria (ThO2) has lately gained attention due to its potential for use as a nuclear fuel. From a physics standpoint, ThO2 is an actinide-bearing material with no 5f electrons and is thus ideally suited as a baseline material for future studies of the physical properties of actinide systems with correlated electrons. Current investigations of ThO2 as a nuclear fuel focus on the influence of radiation-induced lattice defects on its thermal properties, especially the conductivity. This work presents a first investigation of the impact of point defect disorder on phonon thermal conductivity of ThO2 by solving the Boltzmann transport equation within the single-mode relaxation time approximation. The relaxation times of intrinsic, three-phonon scattering are calculated by a rigorous sampling of k-points within the irreducible Brillouin zone of the face-centered cubic crystal structure. The effect of point defects on the thermal conductivity of ThO2 is predicted using the classic model by Klemens for phonon relaxation times that result from the change in mass and induced lattice strain associated with point defects. Within this model, the change in force constants and atomic radii are computed using input from an atomistic model of ThO2. The defects considered are uranium substitution at a thorium site, oxygen vacancies and interstitials, and thorium vacancies and interstitials. The results show that the conductivity of ThO2 is highly sensitive to intrinsic point defects and less sensitive to U substitution on the cation sublattice. [ABSTRACT FROM AUTHOR]
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