Predicting density functional theory total energies and enthalpies of formation of metal-nonmetal compounds by linear regression

Ann M. Deml, Ryan O'Hayre, Chris Wolverton, Vladan Stevanović*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

72 Scopus citations


The availability of quantitatively accurate total energies (Etot) of atoms, molecules, and solids, enabled by the development of density functional theory (DFT), has transformed solid state physics, quantum chemistry, and materials science by allowing direct calculations of measureable quantities, such as enthalpies of formation (ΔHf). Still, the ability to compute Etot and ΔHf values does not, necessarily, provide insights into the physical mechanisms behind their magnitudes or chemical trends. Here, we examine a large set of calculated Etot and ΔHf values obtained from the DFT+U-based fitted elemental-phase reference energies (FERE) approach [V. Stevanović, S. Lany, X. Zhang, and A. Zunger, Phys. Rev. B 85, 115104 (2012)10.1103/PhysRevB.85.115104] to probe relationships between the Etot/ΔHf of metal-nonmetal compounds in their ground-state crystal structures and properties describing the compound compositions and their elemental constituents. From a stepwise linear regression, we develop a linear model for Etot, and consequently ΔHf, that reproduces calculated FERE values with a mean absolute error of ∼80 meV/atom. The most significant contributions to the model include calculated total energies of the constituent elements in their reference phases (e.g., metallic iron or gas phase O2), atomic ionization energies and electron affinities, Pauling electronegativity differences, and atomic electric polarizabilities. These contributions are discussed in the context of their connection to the underlying physics. We also demonstrate that our Etot/ΔHf model can be directly extended to predict the Etot and ΔHf of compounds outside the set used to develop the model.

Original languageEnglish (US)
Article number085142
JournalPhysical Review B
Issue number8
StatePublished - Feb 29 2016

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics


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