Manipulation of molecular vibrational motions via pure rotational excitations

The coupling between different molecular degrees of freedom plays a decisive role in many quantum phenomena, including electron transfer and energy redistribution. Here, we demonstrate a quantum-mechanical time-dependent simulation to explore how a vibrational motion in a molecule can be affected via the rotation-vibration coupling. Our simulations show that a slow (compared to the vibrational period) rotational excitation leads to a smooth increase in the bond length whereas a fast rotational excitation leads to a non-stationary vibrational motion.