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Molecular Orbitals for Excited States

The use of Mulliken's "ionic Hamiltonian" to obtain excited state orbitals is investigated. When compared with the ordinary virtual orbital method it is found to give improved charge distributions for the excited orbitals, but seems to be of less value for improving excitation energies in a minimal-basis calculation. As examples, INDO calculations have been carried out on the ethylene, formaldehyde, and pyridine molecules.