Three-body components of collision-induced absorption

Details Three-body components of collision-induced absorption Three-body components of collision-induced absorption

Dec 1989

adsabs.harvard.edu/cgi-bin/nph-data_query?bibcode=1989phrva..40.6260m&link_type=abstract

Physical Review A (General Physics), Volume 40, Issue 11, December 1, 1989, pp.6260-6274

Physics

Chemical Physics

16

Infrared Spectra, Other Topics In Atomic And Molecular Collision Processes And Interactions, Other Topics In Physical Chemistry And Chemical Physics

Scientific paper

Expressions for the three-body coefficients are derived by virial expansion of the zeroth and first moments of collision-induced spectra. For the ternary supermolecular complexes He-Ar-Ar, He-He-Ar, H2-He-He, H2-H2-He, H2-H2-H2, and H2-Ar-Ar, these are evaluated numerically from first principles at a few temperatures between 50 and 300 K, using the most dependable induced-dipole and intermolecular potential functions available. Both rototranslational and rotovibrational bands are considered. Only the pairwise-additive contributions to the three-body induced-dipole moments are considered. Quantum corrections of the Wigner-Kirkwood type are given and found to be important. Strong three-body spectral components are predicted at the lower temperatures. The computed three-body spectral moments are compared with available laboratory measurements in the near- and far-infrared regions. At temperatures above 50 K, measured ternary moments are found to be consistently greater than calculated ones, especially at the higher temperatures. The excess may be due to a positive ternary spectral component of collision-induced absorption arising from nonadditive induced-dipole components of molecular triplets.

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