Abstract
Frequency dependent second hyperpolarizabilities of N2 and the prototype organic molecule trans-butadiene are reported using generalized time dependent Hartree–Fock (TDHF) theory for several frequencies of applied fields. A monotonic increase of the values (positive dispersion) is observed for every nonlinear optical process in a range of frequencies for the applied field. Correlation effects are estimated using a second-order many body perturbation theory and coupled cluster singles and doubles relaxed density method for the analytical determination of the induced dipole moment. Such hybrid results for DC-induced second harmonic generation provide reasonable values in comparison with experiment for N2. However, dispersion and correlation effects in trans-butadiene are both found to be large and could be nonadditive.
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