Automating firstprinciples phase diagram calculations
 A. van de Walle,
 G. Ceder
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Devising a computational tool that assesses the thermodynamic stability of materials is among the most important steps required to build a “virtual laboratory,” where materials could be designed from first principles without relying on experimental input. Although the formalism that allows the calculation of solidstate phase diagrams from first principles is well established, its practical implementation remains a tedious process. The development of a fully automated algorithm to perform such calculations serves two purposes. First, it will make this powerful tool available to a large number of researchers. Second, it frees the calculation process from arbitrary parameters, guaranteeing that the results obtained are truly derived from the underlying firstprinciples calculations. The proposed algorithm formalizes the most difficult step of phase diagram calculations, namely the determination of the “cluster expanison,” which is a compact representation of the configurational dependence of the alloy’s energy. This is traditionally achieved by a fit of the unknown interaction parameters of the cluster expansion to a set of structural energies calculated from first principles. We present a formal statistical basis for the selection of both the interaction parameters to include in the cluster expansion and the structures to use to determine them. The proposed method relies on the concepts of crossvalidation and variance minimization. An application to the calculation of the phase diagram of the SiGe, CaOMgO, TiAl, and CuAu systems is presented.
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 Title
 Automating firstprinciples phase diagram calculations
 Journal

Journal of Phase Equilibria
Volume 23, Issue 4 , pp 348359
 Cover Date
 20020801
 DOI
 10.1361/105497102770331596
 Print ISSN
 10549714
 Publisher
 SpringerVerlag
 Additional Links
 Topics
 Industry Sectors
 Authors

 A. van de Walle ^{(1)}
 G. Ceder ^{(2)}
 Author Affiliations

 1. Department of Materials Science and Engineering, Northwestern University, 60208, Evanston, IL
 2. Department of Materials Science and Engineering, Massachusetts Institute of Technology, 02139, Cambridge, MA