Density-decomposed orbital-free density functional theory for covalently bonded molecules and materials

Junchao Xia, Emily A. Carter

Research output: Contribution to journalArticlepeer-review

42 Scopus citations


We propose a density decomposition scheme using a Wang-Govind-Carter- (WGC-) based kinetic energy density functional (KEDF) to accurately and efficiently simulate various covalently bonded molecules and materials within orbital-free (OF) density functional theory (DFT). By using a local, density-dependent scale function, the total density is decomposed into a highly localized density within covalent bond regions and a flattened delocalized density, with the former described by semilocal KEDFs and the latter treated by the WGC KEDF. The new model predicts reasonable equilibrium volumes, bulk moduli, and phase-ordering energies for various semiconductors compared to Kohn-Sham (KS) DFT benchmarks. The decomposition formalism greatly improves numerical stability and accuracy, while retaining computational speed compared to simply applying the original WGC KEDF to covalent materials. The surface energy of Si(100) and various diatomic molecule properties can be stably calculated and also agree well with KSDFT benchmarks. This linear-scaled, computationally efficient, density-partitioned, multi-KEDF scheme opens the door to large-scale simulations of molecules, semiconductors, and insulators with OFDFT.

Original languageEnglish (US)
Article number235109
JournalPhysical Review B - Condensed Matter and Materials Physics
Issue number23
StatePublished - Dec 7 2012

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Condensed Matter Physics


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