Controlling the sense of molecular rotation: Classical versus quantum analysis

Recently, it was predicted theoretically and verified experimentally that a pair of delayed and cross-polarized short laser pulses can create molecular ensembles with a well-defined sense of rotation (clockwise or counterclockwise). Here we provide a comparative study of the classical and quantum aspects of the underlying mechanism for linear molecules and for symmetric tops, like benzene molecules, that were used for the first experimental demonstration of the effect. Very good quantitative agreement is found between the classical description of the process and the rigorous quantum-mechanical analysis at the relevant experimental conditions. Both approaches predict the same optimal values for the delay between pulses and the angle between them, and deliver the same magnitude of the induced oriented angular momentum of the molecular ensemble. As expected, quantum and classical analyses substantially deviate when the delay between pulses is comparable with the period of quantum rotational revivals. However, time-averaged characteristics of the excited molecular ensemble are equally well described by these two approaches. This is illustrated by calculating the anisotropic time-averaged angular distribution of the double-pulse excited molecules, which reflects persistent confinement of the molecular axes to the rotation plane defined by two polarization vectors of the pulses.