Simplified DFT methods for consistent structures and energies of large systems. (2nd May 2018)

• Record Type: Journal Article
• Authors: Caldeweyher, Eike; Brandenburg, Jan Gerit
• Is Part Of: Journal of physics. Volume 30:Number 21(2018)
• Publication Date: 2018-05-02
• Subjects: density functional theory -- London dispersion -- molecular crystal -- lattice energy -- basis set expansion -- non-covalent interaction; Condensed matter -- Periodicals; Matière condensée -- Périodiques; Vaste stoffen; Vloeistoffen; Natuurkunde; Electronic journals; Computer network resources; 530.4105
• DOI: 10.1088/1361-648X/aabcfb
• Languages: English
• ISSNs: 0953-8984

Abstract

Abstract: Kohn–Sham density functional theory (DFT) is routinely used for the fast electronic structure computation of large systems and will most likely continue to be the method of choice for the generation of reliable geometries in the foreseeable future. Here, we present a hierarchy of simplified DFT methods designed for consistent structures and non-covalent interactions of large systems with particular focus on molecular crystals. The covered methods are a minimal basis set Hartree–Fock (HF-3c), a small basis set screened exchange hybrid functional (HSE-3c), and a generalized gradient approximated functional evaluated in a medium-sized basis set (B97-3c), all augmented with semi-classical correction potentials. We give an overview on the methods design, a comprehensive evaluation on established benchmark sets for geometries and lattice energies of molecular crystals, and highlight some realistic applications on large organic crystals with several hundreds of atoms in the primitive unit cell.