Direct imaging of rotational wave-packet dynamics of diatomic molecules

Control of rotational wave-packet dynamics in asymmetric top molecules

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 struc...

Rotational Spectroscopy of Diatomic Molecules

Rotational structures of long-range diatomic molecules

We present a systematic understanding of the rotational structure of a long-range (vibrationally highly-excited) diatomic molecule. For example, we show that depending on a quantum defect, the leastbound vibrational state of a diatomic molecule with −Cn/r (n > 2) asymptotic interaction can have only 1, 2, and up to a maximum of n − 2 rotational levels. A classification scheme of diatomic molecu...

Dynamics of the rotational degrees of freedom in a supercooled liquid of diatomic molecules

Using molecular dynamics computer simulations, we investigate the dynamics of the rotational degrees of freedom in a supercooled system composed of rigid, diatomic molecules. The interaction between the molecules is given by the sum of interaction-site potentials of the Lennard-Jones type. In agreement with mode-coupling theory (MCT), we find that the relaxation times of the orientational time ...

Oriented rotational wave-packet dynamics studies via high harmonic generation.

We produce oriented rotational wave packets in CO and measure their characteristics via high harmonic generation. The wave packet is created using an intense, femtosecond laser pulse and its second harmonic. A delayed 800 nm pulse probes the wave packet, generating even-order high harmonics that arise from the broken symmetry induced by the orientation dynamics. The even-order harmonic radiatio...