From Electronic Structure to Thermodynamics of Actinide-Based Alloys

In this brief review, we show that thermodynamic modeling of complex multicomponent actinide-based alloys is crucial for fuel development and for predicting the impact of evolving fuel chemistry with time on materials performance. With input from energetics and equilibrium properties of alloys from ab initio electronic-structure calculations, within the framework of density-functional theory, the CALPHAD methodology is a viable approach to thermodynamic assessment for this class of materials. Despite the limited availability of experimental thermodynamic data, this approach can predict important features in the phase diagram and, perhaps more importantly, guide and motivate further experiments for validating the methodology and the data for subsequent modeling of materials performance on a higher level.