Wave‐function‐based ab initio correlation treatment for the buckminsterfullerene C 60

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. © 2004 Wiley Periodicals, Inc. Int J Quantum Chem, 2004