Correlation potentials and functionals in Hartree-Fock-Kohn-Sham theory

Abstract
We compute molecular Hartree-Fock-Kohn-Sham correlation potentials from ab initiocoupled-cluster densities via a modified Zhao, Morrison and Parr [Phys. Rev. A, 50, (1994) 2138] scheme involving exact exchange. We examine the potential for several small systems, and observe complex structure. By fitting a functional expansion to our potentials we obtain a closed-shell functional which is an improvement over other pure correlationfunctionals in Hartree-Fock-Kohn-Sham calculations. The leading term in our functional is dependent on the number of electrons. Our results lead us to question the utility of correlation defined within the Hartree-Fock-Kohn-Sham scheme, and to consider alternative partitionings of the exchange-correlation energy.