Theory of second-harmonic generation of molecular systems: The case of coincident pulses

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Abstract
While, for a long time, steady-state second-harmonic generation has provided important information concerning optical nonlinearities and dynamics of molecular systems, either isolated or adsorbed, time-resolved measurements are now becoming very productive. It is the aim of the present work to introduce a theoretical model of time-resolved second-harmonic generation involving a detailed description of the electronic and vibrational structures of the molecular system. It will be of interest to obtain a better understanding of the dynamics taking place in these systems in terms of their internal parameters.