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• W1582335547 startingPage "169" @default.
• W1582335547 abstract "Vibrational relaxation of the 61 level of S1(1B2u) benzene is analyzed using the angular momentum model of inelastic processes. Momentum–(rotational) angular momentum diagrams illustrate energetic and angular momentum constraints on the disposal of released energy and the effect of collision partner on resultant benzene rotational excitation. A kinematic “equivalent rotor” model is introduced that allows quantitative prediction of rotational distributions from inelastic collisions in polyatomic molecules. The method was tested by predicting K-state distributions in glyoxal–Ne as well as J-state distributions in rotationally inelastic acetylene–He collisions before being used to predict J and K distributions from vibrational relaxation of 61 benzene by H2, D2, and CH4. Diagrammatic methods and calculations illustrate changes resulting from simultaneous collision partner excitation, a particularly effective mechanism in p-H2 where some 70% of the available 61→00 energy may be disposed into 0→2 rotation. These results support the explanation for branching ratios in 61→00 relaxation given by Waclawik and Lawrance and the absence of this pathway for monatomic partners. Collision-induced vibrational relaxation in molecules represents competition between the magnitude of the energy gap of a potential transition and the ability of the colliding species to generate the angular momentum (rotational and orbital) needed for the transition to proceed. Transition probability falls rapidly as ΔJ increases and for a given molecule–collision partner pair will provide a limit to the gap that may be bridged. Energy constraints increase as collision partner mass increases, an effect that is amplified when Ji&gt;0. Large energy gaps are most effectively bridged using light collision partners. For efficient vibrational relaxation in polyatomics an additional requirement is that the molecular motion of the mode must be capable of generating molecular rotation on contact with the collision partner in order to meet the angular momentum requirements. We postulate that this may account for some of the striking propensities that characterize polyatomic energy transfer." @default.
• W1582335547 created "2016-06-24" @default.
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• W1582335547 date "2004-06-18" @default.
• W1582335547 modified "2023-09-27" @default.
• W1582335547 title "The role of angular momentum in collision-induced vibration–rotation relaxation in polyatomics" @default.
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• W1582335547 doi "https://doi.org/10.1063/1.1758696" @default.
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