Analysis of the two-photon absorption spectrum of benzonitrile based on the direct quantum-mechanical calculation of the intensity distribution.

A direct quantum-mechanical calculation of the intensity distribution in the two-photon absorption spectrum of benzonitrile is performed taking into account the Herzberg-Teller effect. The excitation mechanism of all the observed lines, including lines corresponding to the excitation of single-quantum nontotally symmetric vibrations and their combinations with totally symmetric modes, is analyzed. The results of the calculation, performed taking into account the frequency effect and the Duschinsky effect, agree satisfactorily with experimental data. This indicates that it is worthwhile to apply the quantum-mechanical method in calculations of the intensity distribution in the two-photon absorption spectra of cyclic molecules. [ABSTRACT FROM AUTHOR]