Calculation of the third-order nonlinear optical response Of nitrobenzene

Measurement of the third-order response of materials can provide much useful information about the molecular dynamics governing other macroscopic properties. Currently, attention is focused on obtaining such data via time domain measurements (pump-probe technique). While such measurements can give a phenomenological understanding of the mechanisms of the excitations, they allow little or no comparison to theoretical predictions. The present paper addresses this problem by performing a frequency domain analysis of the third-order response of a convenient model system, liquid nitrobenzene. Theoretical predictions are then compared to data from an induced birefringence measurement.