Echo Spectroscopy in Multilevel Quantum-Mechanical Rotors

We study the dynamics of rotational echoes in gas phase molecular ensembles and their dependence on the delay and intensity of the excitation pulses. We explore the unique dynamics of alignment echoes that arise from the multilevel nature of the molecular rotors and impose severe difficulties in utilizing echo responses for rotational spectroscopy. We show experimentally and theoretically that judicious control of both the delay and intensity of the second pulse enables multilevel "rotational echo spectroscopy." The proposed methodology paves the way to rotational spectroscopy in high-density gas samples.