A quantal description of the response of an extended molecular system to external probes is developed in terms of collision time-correlation functions. The system is partitioned into a primary region, where localized excitations occur, and a secondary region surrounding it. A time-dependent self-consistent field procedure is followed to derive coupled quantal equations for the transition amplitudes in both regions, and a general model is introduced for cases where the secondary region undergoes harmonic motions. A numerical procedure based on path integrals, obtained for complex times by a sequence of matrix multiplications, is illustrated with calculations of cross sections for photodissociation of CH3I. © 1990.
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