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Automating first-principles phase diagram calculations

van de Walle, A. and Ceder, G. (2002) Automating first-principles phase diagram calculations. Journal of Phase Equilibria, 23 (4). pp. 348-359. ISSN 1054-9714. doi:10.1361/105497102770331596.

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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 solid-state 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 first-principles 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 cross-validation and variance minimization. An application to the calculation of the phase diagram of the Si-Ge, CaO-MgO, Ti-Al, and Cu-Au systems is presented.

Item Type:Article
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van de Walle, A.0000-0002-3415-1494
Additional Information:© 2002 Springer Verlag. Submitted 24 September 2001. This work was supported by the U.S. Department of Energy, Office of Basic Energy Sciences, under contract no. DE-F502-96ER 45571. Gerbrand Ceder acknowledges support of Union Minière through a Faculty Development Chair. Axel van de Walle acknowledges support of the National Science Foundation under program DMR-0080766 during his stay at Northwestern University.
Funding AgencyGrant Number
Department of Energy (DOE) Office of Basic Energy SciencesDE-F502-96ER 45571
Union Minière Faculty Development ChairUNSPECIFIED
Issue or Number:4
Record Number:CaltechAUTHORS:20111031-152105270
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:27535
Deposited By: Tony Diaz
Deposited On:01 Nov 2011 21:06
Last Modified:09 Nov 2021 16:49

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