Nonlocal potentials for short-range electronic correlation in atoms, molecules, and solids

TL;DR

This paper develops a new methodology for nonlocal exchange and correlation potentials in density functional theory, enabling ab initio orbital functional calculations for atoms, molecules, and solids.

Contribution

It introduces modifications to a standard atomic program and extends UHF theory with a Colle-Salvetti Ansatz for short-range correlation, applicable to complex systems.

Findings

Results for atoms He-Ne demonstrate the method's effectiveness.

Parameters for molecules and solids are provided.

Discussion on implementing nonlocal potentials in extended systems.

Abstract

Extending density functional theory (DFT) to an {\it ab initio} orbital functional theory (OFT) requires new methodology for nonlocal exchange and correlation potentials. This paper describes such modifications to a standard Dirac-Slater atomic program. Unrestricted Hartree-Fock (UHF) theory is extended by a modified Colle-Salvetti Ansatz for short-range electronic correlation. Results are reported for atoms He-Ne. Values of parameters needed for similar calculations on molecules and solids are reported. Implementation of nonlocal exchange and correlation for such extended systems, using multiple scattering theory to connect independent calculations in space-filling atomic cells, is discussed.