Control of rotational wave-packet dynamics in asymmetric top molecules

Abstract

We combine newly developed experimental and theoretical methods to explore and control the rotations of asymmetric top molecules. In the low-temperature limit, the revival spectra of laser-driven rotational wave packets exhibit a fascinating quantum-mechanical structure, which is qualitatively different for asymmetric tops compared to symmetric or linear tops. With increasing fluence, the structure gradually simplifies, illustrating a controllable transformation of the rotational dynamics. Our theoretical and experimental predictions are in qualitative agreement.