Chemical short-range-order effects on stability in δ-Pu–Ga alloys

Abstract

We present results on the structural stability of Pu_{1− x} Ga _x alloys based on the local spin-density approximation and including non-local corrections to the exchange–correlation functional (generalized gradient approximation). First, we used both the linearized augmented plane-wave and the projector augmented wave (PAW) methods to calculate the energies of formation of five intermediate phases which occur in the Pu–Ga phase diagram. Then, PAW calculations were performed for various superstructures based on the fcc lattice to get the interaction parameters to describe the energetics of the δ-Pu–Ga solid solution. To discuss the effects of the chemical short-range order on the structural stability of the δ-Pu–Ga solid solution as a function of temperature, the cluster variation method configurational entropy has been introduced using the regular tetrahedron approximation. The solid part of the Pu-rich side of the phase diagram involving phase equilibria between the Pu phases, the δ-Pu–Ga solid solution and the Pu₃Ga compound is calculated. We show the importance of chemical short-range order on Ga solubility in δ-Pu.

Acknowledgements

This work was supported by computer grant 21513 of the Institut du Développement et des Ressources en Informatique Scientifique (IDRIS). An allocation on PHYsique NUMérique is also greatly acknowledged.