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Time dependent thermal lensing measurements of V -- T energy transfer from highly excited NO sub 2

Journal Article · · Journal of Chemical Physics; (USA)
DOI:https://doi.org/10.1063/1.458573· OSTI ID:7002874
; ;  [1]
  1. Department of Atmospheric, Oceanic, University of Michigan, Ann Arbor, Michigan 48109-2143 (USA) Space Sciences, Space Physics Research Laboratory, The University of Michigan, Ann Arbor, Michigan 48109-2143 (USA)

The time dependent thermal lensing technique has been used to measure the vibrational relaxation of NO{sub 2} (initially excited at 21 631 cm{sup {minus}1}) by Ar, Kr, and Xe. The energy transfer analysis was carried out in terms of {l angle}{l angle}{Delta}{ital E}{r angle}{r angle}, the bulk average energy transferred per collision. This quantity was found to have a very strong dependence on vibrational energy, with a marked increase at energies greater than about 10 000 cm{sup {minus}1}, where several electronic excited states ({sup 2}{ital B}{sub 2}, {sup 2}{ital B}{sub 1}, and {sup 2}{ital A}{sub 2}) mix with the ground state ({sup 2}{ital A}{sub 1}). This effect may be due to large amplitude vibrational motions associated with the coupled electronic states. Even at low energies, deactivation is faster than in other triatomic systems, probably because NO{sub 2} is an open shell molecule and electronic curve crossings provide efficient pathways for vibrational deactivation. The {ital V}--{ital T} rate constant for deactivation of NO{sub 2}(010) by argon is estimated to be (5.1{plus minus}1.0){times}10{sup {minus}14} cm{sup 3} s{sup {minus}1}. Results obtained for NO{sup *}{sub 2}--NO{sub 2} collisions gave {l angle}{l angle}{Delta}{ital E}{r angle}{r angle} values in good agreement with literature results from fluorescence quenching experiments, indicating that {ital V}--{ital T} may be more important than {ital V}--{ital V} energy transfer in the quenching process.

OSTI ID:
7002874
Journal Information:
Journal of Chemical Physics; (USA), Journal Name: Journal of Chemical Physics; (USA) Vol. 92:8; ISSN JCPSA; ISSN 0021-9606
Country of Publication:
United States
Language:
English