Nonlinear response functions for birefringence and dichroism measurements in condensed phases

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Abstract
The fourth-rank tensorial nonlinear response function which controls the response of a chromophore in the condensed phase to three arbitrarily polarized external fields is calculated. Internal (vibrational and rotational) degrees of freedom are incorporated using wave packets in Liouville space (the doorway/window picture). The rotational contribution of the chromophore is expressed in terms of a conditional probability for the rotational diffusion model. We apply this formalism to transient dichroism and birefringence spectroscopies.