TREATMENT OF ELECTRONIC EXCITATIONS WITHIN THE ADIABATIC APPROXIMATION OF TIME-DEPENDENT DENSITY-FUNCTIONAL THEORY

Time dependent density functional methods are applied in the adiabatic approximation to compute low-lying electronic excitations of N-2, eth ylene, formaldehyde, pyridine and porphin. Out of various local, gradi ent-corrected and hybrid (including exact exchange) functionals, the b est results are obtained for the three-parameter Lee-Yang-Parr (B3LYP) functional proposed by Becke. B3LYP yields excitation energies about 0.4 eV too low but typically gives the correct ordering of states and constitutes a considerable improvement over HF-based approaches requir ing comparable numerical work.