IR Laser Excitation in Molecules: Chaos and Diffusive Energy Growth
After a short review of a generic vibrational model of IR multiple-photon excitation, we generalize the model to include rotations. It is shown that the combination of chaotic dynamics and rotational averaging leads to fluence-dependent absorption which removes the sensitivity of the results to model-dependent parameters. The classical rotation-vibration dynamics observed in this model correlate very well with one’s quantum intuition based on a molecule’s P, Q and R-branch structure and on the red-shift of the vibrational absorption with excitation. The implication of these results for MPE experiments is discussed.
KeywordsMicrowave Coherence Mandel
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