The interaction of carbonyl sulfide dipolar gas molecules with two time-delayed, single-cycle THz pulses is shown both experimentally and theoretically to induce two-quantum rotational coherences that are significantly enhanced with respect to those induced by one THz pulse, depending on the relative delay of the pulses. The underlying phenomenon is quite general in that it can occur even after a single THz pulse if more than one molecular species is present, since the free induction decay emitted by one species (demonstrated here by atmospheric water vapor) can provide the second field interaction for the other.

• Received 14 April 2012

DOI:https://doi.org/10.1103/PhysRevLett.109.123603