CARBON DIOXIDE - LASER INDUCED IER AND CHEMISTRY OF CHROMYL CHLORIDE.
Item
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Title
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CARBON DIOXIDE - LASER INDUCED IER AND CHEMISTRY OF CHROMYL CHLORIDE.
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Identifier
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AAI8312364
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identifier
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8312364
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Creator
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NIEMAN, JAIME.
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Contributor
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A. M. Ronn
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Date
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1983
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Language
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English
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Publisher
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City University of New York.
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Subject
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Chemistry, Physical
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Abstract
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High order CO(,2)-laser multiphoton excitation in the ground electronic state of collision-free CrO(,2)Cl(,2) 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. A theoretical model based on this description is analyzed. It is shown that the long radiative lifetime of the observed CrO(,2)Cl(,2) emission is consistent with this interpretation. Molecular requirements for observation of this novel reverse internal conversion process in other molecular systems are suggested.;The fluorescent channel is shown to compete with a dissociative channel forming CrO(,2)Cl + Cl; the radical further dissociates to the stable product CrO(,2). The threshold for fluorescence versus dissociation is discussed and a branching ratio, and a consequent chemical mechanism is suggested. The molecular and laser parameters involved in this competition are also discussed within the framework of the accepted model of infrared multiphoton excitation.
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Type
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dissertation
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Source
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PQT Legacy CUNY.xlsx
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degree
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Ph.D.
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Program
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Chemistry
