Abstract
We demonstrate the observation of quasiperiodic revivals out to 27 ps in an impulsively aligned asymmetric-top molecule, sulfur dioxide , at high sample temperature and density (295 K, 0.5 bar). We find that the asymmetric top exhibits a strong correlation between population alignment and population lifetime , in accordance with the trend observed in linear molecules. We use a linear birefringence measurement fit to a full quantum simulation of the asymmetric rotor and are able to separately measure both the population and coherence lifetimes of the rotational wave packet. Additionally, we observe a high rate of elastic decoherence and attribute this to long-range interactions mediated by the permanent dipole of the molecule. We propose the use of birefringence measurements to study intermolecular interactions in a coherent ensemble, as a step toward using field-free alignment to investigate reaction dynamics and dissipative processes.
- Received 26 November 2015
DOI:https://doi.org/10.1103/PhysRevA.93.013421
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