Abstract
We give details of the spectroscopic observation of the gyroscopic destabilisation in the ν23 vibrational state of dimethylsulfoxide (DMSO) announced by Cuisset, Pirali, and Sadovskií [Phys. Rev. Lett. 109, 094101 (2012)]. Following the first successful high-resolution spectroscopic study of the rotational structure of the "perpendicular" band of DMSO at 324 cm(-1) associated with the ν23 bending vibrational mode, the rare subsystem of ν23 rotational levels consisting of a series of fourfold quasidegenerate levels (4-clusters) was identified. Our complete analysis of the underlying rotational dynamics uncovered a bifurcation leading to the gyroscopic destabilisation of one of the two stable principal axes of inertia, a phenomenon known previously only in a few triatomic molecules.
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