Abstract:The quadratic optical susceptibility of molecular crystals is calculated in the frequency region of vibronic excitations consisting of an electronic exciton and a non-totally symmetric vibration. An one-dimensional model with nearest-neighbour interactions is used. Intermolecular and intramolecular exciton-phonon interactions are considered and the former is shown to play a dominant role in nonlinear optical spectra. The sign of the exciton effective mass is shown to affect the spectrum inside the two-particle… Show more
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