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Vibration. -->. vibration energy transfer in methane

Journal Article · · J. Chem. Phys.; (United States)
DOI:https://doi.org/10.1063/1.438970· OSTI ID:5319299

Vibrational energy levels of methane in the range 2800 to 6000 cm/sup -1/ were excited by a pulsed tunable laser. Infrared fluorescence decays were observed at 294 K and analyzed to yield V..-->..V energy transfer pathways and rates. Symmetric stretching excitation is converted to asymmetric stretching in the same molecule with a rate constant k/sub 1/3.6=(plus-or-minus0.9) x 10/sup -11/ cm/sup 3/ molecule/sup -1/ s/sup -1/ (P=0.09). The ..nu../sub 2/ and ..nu../sub 4/ bending vibrations are interconverted somewhat less rapidly. Stretching excitation is converted to bending with a rate constant of (0.8 +- 0.2) x 10/sup -11/ cm/sup 3/ molecule/sup -1/ s/sup -1/ (P=0.022) for the stretching fundamentals and about twice that for overtone or combination levels. The rate of almost exactly resonant transfer of a vibrational quantum from one molecule to another was about (1.8 +- 0.6) x 10/sup -11/ cm/sup 3/ molecule/sup -1/ s/sup -1/ (P=0.05) for transfer of a bending quantum from CH/sub 4/(2..nu../sub 4/) and about three times less for transfer of a stretching quantum.

Research Organization:
Department of Chemistry, University of California, Berkeley, California 94720
DOE Contract Number:
W-7405-ENG-48
OSTI ID:
5319299
Journal Information:
J. Chem. Phys.; (United States), Journal Name: J. Chem. Phys.; (United States) Vol. 72:10; ISSN JCPSA
Country of Publication:
United States
Language:
English