We report on laser trapping and unidirectional angular acceleration of CO2 molecules to energies well beyond the ground state C-O bond dissociation energy. While a centrifugal dissociation barrier prevents prompt dissociation of these molecules, coherent Raman probing, and virtually imaged phased array (VIPA) detection of the scattering signals, provides direct evidence of coherence transfer and rotation-to-vibration energy transfer. The record-breaking acceleration of CO2 to J=364, corresponding to a rotational temperature of over 71,000 K, and high-resolution detection method permitted the determination of improved centrifugal distortion constants.
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