Effects of Ultrafast Molecular Rotation on Collisional Decoherence

Using an optical centrifuge to control molecular rotation in an extremely broad range of angular momenta, we study coherent rotational dynamics of nitrogen molecules in the presence of collisions. We cover the range of rotational quantum numbers between J = 8 and J = 66 at room temperature and study a crossover between the adiabatic and nonadiabatic regimes of rotational relaxation, which cannot be easily accessed by thermal means. We demonstrate that the rate of rotational decoherence changes by more than an order of magnitude in this range of J values and show that its dependence on J can be described by a simplified scaling law.