Journal article
Communication: creation of molecular vibrational motions via the rotation-vibration coupling
Building on recent advances in the rotational excitation of molecules, we show how the effect of rotation-vibration coupling can be switched on in a controlled manner and how this coupling unfolds in real time after a pure rotational excitation. We present the first examination of the vibrational motions which can be induced via the rotation-vibration coupling after a pulsed rotational excitation.
A time-dependent quantum wave packet calculation for the HF molecule shows how a slow (compared to the vibrational period) rotational excitation leads to a smooth increase in the average bond length whereas a fast rotational excitation leads to a non-stationary vibrational motion. As a result, under field-free postpulse conditions, either a stretched stationary bond or a vibrating bond can be created due to the coupling between the rotational and vibrational degrees of freedom.
The latter corresponds to a laser-induced breakdown of the adiabatic approximation for rotation-vibration coupling.
Language: | English |
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Publisher: | AIP Publishing LLC |
Year: | 2015 |
Pages: | 221101 |
ISSN: | 10897690 and 00219606 |
Types: | Journal article |
DOI: | 10.1063/1.4922309 |
ORCIDs: | Henriksen, Niels Engholm |