First principles thermodynamical modeling of the binodal and spinodal curves in lead chalcogenides.

ABSTRACT

High-throughput ab initio calculations, cluster expansion techniques, and thermodynamic modeling have been synergistically combined to characterize the binodal and the spinodal decompositions features in the pseudo-binary lead chalcogenides PbSe-PbTe, PbS-PbTe, and PbS-PbSe. While our results agree with the available experimental data, our consolute temperatures substantially improve with respect to previous computational modeling. The computed phase diagrams corroborate that in ad hoc synthesis conditions the formation of nanostructure may occur justifying the low thermal conductivities in these alloys. The presented approach, making a rational use of online quantum repositories, can be extended to study thermodynamical and kinetic properties of materials of technological interest.