Wave-function-based ab initio correlation treatment for the buckminsterfullerene C60

First-principle calculations for large extended systems such as the buckminsterfullerene C-60 are mainly performed within density functional theory. They yield reasonable agreement with experiment, but wave-function-based correlations methods are preferable to obtain better insight into the correlation properties. Starting from a Hartree-Fock calculation for the solid, an incremental scheme relying on localized orbitals is developed for the correlation energy of C-60. This many-body expansion converges well with distance of localized bonds involved in the correlation methods and with order of increments. A detailed knowledge of the influence of the correlation effects on the binding and the bond alternation is achieved. Comparison with diamond, graphite, and polyacetylene is made. (C) 2004 Wiley Periodicals, Inc.