Abstract

Quantum dynamical theory of molecular Fermi resonance (va,2vb) based on a model of two non-linearly coupled oscillators is developed. A time-dependent solution for the population of the vibrational modes in terms of elliptic functions is obtained. It is shown that the period of the intramolecular energy exchange is simply connected with the anharmonic potential constant. To substantiate the author's theoretical results subpicosecond pump and probe techniques and a new method of time-resolved spectroscopy without requiring ultrashort pulses may be used. The period of the energy exchange, the potential constant and the frequency difference of a Fermi doublet may be directly determined from the proposed experiments.

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