1 February 1980 Multiphoton Induced Inverse Electronic Relaxation
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High order infrared multiphoton excitation in the ground electronic state of collision free CrO2Cl2 has resulted in visible fluorescence. The prompt fluorescence has been studied as a function of laser fluence, pulse duration, under collisional and collision-free conditions and was shown to arise from a spontaneous one-photon radiative decay of molecular eigenstates. Intramolecular scrambling of vibronic levels corresponding to the ground state electronic manifold with a discrete level(s) belonging to the low lying excited electronic state is believed to be the origin of such eigenstates. This fluorescent channel is shown to compete with a dissociative channel forming CrO2Cl + CI; the radical further dissociates to the stable product Cr02. The threshold for fluorescence versus dissociation is discussed and a branching ratio, and consequent chemical mechanism are suggested.
J. Nieman, A. M. Ronn, "Multiphoton Induced Inverse Electronic Relaxation," Optical Engineering 19(1), 191039 (1 February 1980). https://doi.org/10.1117/12.7972467 . Submission:

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