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A time-dependent formulation of two-photon spectroscopy is employed to show that selectivity of reactivity can be achieved via coherent two-photon processes. The problem of finding the optimum waveform (i.e., coherent pulse sequence) that will maximize the formation of a desired chemical species is formulated as a problem in the calculus of variations, and solved for two different cases.
Tannor et al. (Fri,) studied this question.