The total infrared fluorescence excitation spectrum in the region of the 101→212 rotational transition in the aldehyde C–H stretch fundamental band of methyl formate has been measured with a resolution of ∼0.007 cm−1. Five peaks were observed, indicating that the zeroth order optically active rovibrational state is mixed with nearly isoenergetic optically inactive bath states. This study marks the first use of a single mode optical parametric oscillator (OPO) for a spectroscopic experiment, and it demonstrates a technique with the potential to probe the vibrational makeup of individual molecular eigenstates.
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Minton et al. (1988) studied this question.
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