First-principles calculation study on phonon thermal conductivity of thorium and plutonium dioxides; Intrinsic anharmonic phonon-phonon and extrinsic grain-boundary-phonon scattering effects

Nakamura, Hiroki  ; Machida, Masahiko  

Thermal conductivity of nuclear fuel materials is one of the most essential thermophysical data in analyzing nuclear reactor safety and fuel performance. To establish a reliable technique of computation of their thermal conductivity, we apply a scheme based on first-principles electronic calculations and calculate phonon thermal conductivity of both plutonium and thorium dioxides. In the employed scheme, all phonon properties are calculated from harmonic and third-order anharmonic force constants obtained through first-principles calculations. Using these phonon properties, phonon thermal conductivity are computed with a standard phonon transport theory. The calculation results show a good agreement with experiments. Moreover, we evaluate grain-boundary effects on phonon thermal conduction. These results prove that the present first-principles scheme is reliably applicable to accurate computation of phonon thermal conductivity of fuel materials in the considered temperature range.