Thermal conductivity of non-stoichiometric americium oxide: A molecular dynamics study

The aim of this paper is to investigate the influence of multi-valency of americium in its oxide for the lowering of the thermal conductivity and the uncertainty in measurement. In the present study, thermal conductivity of non-stoichiometric americium oxide was evaluated up to 2000 K by the non-equilibrium molecular dynamics calculations using the Born-Mayer-Huggins interatomic potential with the partially ionic model. The oxygen-to-americium ratio (O/Am) was varied from 1.6 to 1.9, which corresponded to the variation of the ratio of Am³⁺/Am⁴⁺. So, we prepared potential parameters for both Am³⁺ and Am⁴⁺. The calculated thermal conductivity of non-stoichiometric americium oxide decreased with an increase of temperature, and the degree of the temperature dependence became smaller with a decrease of the O/Am ratio. This was mainly caused by the phonon-scattering due to oxygen vacancies induced with Am³⁺ ions. Comparing two supercells in which (1) short-range ordered Am³⁺ clusters were contained and (2) Am³⁺ ions were randomly distributed, the thermal conductivity of the former seemed to be somewhat larger than that of the latter.