Abstract-Coherent radiative decay of molecular rotations: A comparative study of terahertz-oriented versus optically aligned molecular ensembles

Ran Damari, Dina Kardash, and Sharly Fleischer

https://journals.aps.org/prl/accepted/90075Yf2P8d1ac6aa19a48d1ab735de1d94fead04

The decay of field-free rotational dynamics is experimentally studied by two complementary methods: laser-induced molecular alignment and terahertz-field-induced molecular orientation. Comparison between the decay rates of different molecular species at various gas pressures reveals that oriented molecular ensembles decay faster than aligned ensembles. The discrepancy in decay rates is attributed to the coherent radiation emitted by the transiently oriented ensembles and is absent from aligned molecules. The experimental results reveal the dramatic contribution of coherent radiative emission to the observed decay of rotational dynamics and underline a general phenomenon expected whenever field-free coherent dipole oscillations are induced.