ELECTRONIC ENERGIES, DIPOLE-MOMENT MATRIX-ELEMENTS, AND STATIC POLARIZABILITIES AND HYPERPOLARIZABILITIES FOR SOME DIPHENYL MOLECULES

The ''giant dipole'' molecules, NR1R2-C6H4-(C=C)n-C6H4-NO2, n = 0, 1, 2, are studied theoretically for three sets of substituents: R1 = R2 = H, R1 = H, R2 = CH3, and R1 = R2 = CH3. For each of these nine molecu les, the energies, and permanent and transition dipole moments for the 20 lowest electronic states are calculated using the intermediate neg lect of differential overlap (INDO) approximation at the configuration interaction with single excitations (CIS) level. Static polarizabilit ies and hyperpolarizabilities for the ground states are reported for t hese ''push-pull'' molecules. The changes in the physical properties o f interest due to increase in conjugation length and the inductive eff ect of substituents on the donor group attached to the rings are discu ssed. The energies and permanent and transition dipole moments for the ten lowest electronic states are tabulated for use in future studies of the spectral and dynamical effects of permanent dipole moments on l aser-induced one- and multi-photon electronic transitions in realistic models for many-level giant dipole molecules.