Abstract

We report the sub-picosecond time-resolved nonlinear optical properties of poly-DCH single crystal from near resonance to on resonance. The magnitude of the third-order nonlinear susceptibilities of poly-DCH for polarization along the main chain direction were found to be of the order 10-6esu on resonance and 10-7esu near resonance. A photo- induced absorptive nonlinearity was found near resonance and an absorption saturation was found on resonance. The sign change in the imaginary susceptibility is due to the mixing of two phenomena, the free exciton level satutation and the reabsorption of the self-trapped exciton. The self-trapped exciton lifetime was observed to be 1.5-2.3ps near resonance.

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