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Three-level and four-level infrared-infrared double resonance spectroscopy in CH[sub 3]F

Thesis/Dissertation ·
OSTI ID:7114294
A series of three-level and four-level infrared-infrared (IR-IR) double resonance experiments have been carried out to study saturation spectroscopy, to determine the various features of collisionally-induced transitions, to determine the vibration rotation energies of a highly excited vibration state, and to measure the precise frequencies of rovibrational transitions in methyl fluoride. In these experiments, either a fundamental rovibrational transition, or a hot band transition in the [nu][sub 3] vibrational mode of CH[sub 3]F was pumped by a CO[sub 2] laser coincidence, while rovibrational transitions, involving excitation of either the [nu][sub 3] or the [nu][sub 6] vibrational mode, were probed by an infrared microwave sideband laser system. Dynamic Stark splitting (Rabi splitting) has been observed in three-level IR-IR double resonance in CH[sub 3]F. The line shape has been fit to theoretical expressions that were derived from a semi-classical treatment of a three-level system. A very good agreement between theory and experiment has been obtained. Rotation and vibration-rotation transitions in CH[sub 3]F induced by collision with foreign gases such as H[sub 2], He, Ar, Xe or isotopically-labeled CH[sub 3]F have been studied by the method of four-level IR-IR double resonance. All of the observed transitions obey selection rules. It has been found that Ar or Xe can collisionally-induce direct vibrational transitions in CH[sub 3]F more readily than CH[sub 3]F itself. Classical elastic scattering theory has been used to calculate one-dimensional collision kernels with Lennard-Jones and Buckingham-Slater intermolecular potential functions. Initial velocity dependence of the collisionally-induced rotational energy transfer in CH[sub 3]F has been studied.
Research Organization:
Michigan State Univ., East Lansing, MI (United States)
OSTI ID:
7114294
Country of Publication:
United States
Language:
English