Control of Molecular Rotation with a Chiral Train of Ultrashort Pulses

Trains of ultrashort laser pulses separated by the time of rotational revival (typically, tens of picoseconds) have been exploited for creating ensembles of aligned molecules. We introduce a chiral pulse train - a sequence of linearly polarized pulses with the polarization direction rotating from pulse to pulse by a controllable angle. The chirality of such a train, expressed through the period and direction of its polarization rotation, is used as a new control parameter for achieving selectivity and directionality of laser-induced rotational excitation. The method employs chiral trains with a large number of pulses separated on the time scale much shorter than the rotational revival (a few hundred femtosecond), enabling the use of conventional pulse shapers.