2008/04/07 by Balázs Hetényi, Balazs Hetenyi, Andreas Hauser +1
Chemistry · Physics and Astronomy · #Advanced Chemical Physics Studies #Advanced Physical and Chemical Molecular Interactions #Spectroscopy and Quantum Chemical Studies #cond-mat.mtrl-sci #cond-mat.other
paper · pdf · doi:10.1103/physrevb.77.155110
published as Phys. Rev. B 77, 155110 (2008) · to appear in Physical Review B
arxiv created 2008/04/07 · openalex publication_date 2008/04/09 · arxiv updated 2009/12/01 · openalex created_date 2025/10/10 · openalex updated_date 2026/07/28
A practical electronic structure method in which a two-body functional is the fundamental variable is constructed. The basic formalism of our method is equivalent to Hartree-Fock density matrix functional theory [M. Levy, in Density Matrices and Density Functionals, edited by R. Erdahl and V. H. Smith, Jr. (Reidel, Dordrecht, 1987)]. The implementation of the method consists of solving Hartree-Fock equations and using the resulting orbitals to calculate two-body corrections to account for correlation. The correction terms are constructed so that the energy of the system in the absence of external potentials can be made to correspond to approximate expressions for the energy of the homogeneous electron gas. In this work, the approximate expressions we use are based on the high-density limit of the homogeneous electron gas. Self-interaction is excluded from the two-body functional itself. It is shown that our pair density based functional does not suffer from the divergence present in many density functionals when homogeneous scaling is applied. Calculations based on our pair density functional lead to quantitative results for the correlation energies of atomic test cases.