DEVELOPMENT OF A FREQUENCY-SWITCHED LASER FOR INFRARED TIME RESOLVED SPECTROSCOPY.

Abstract

The objective of this thesis is to describe the development, construction and use of a new tool for optical coherent transient spectroscopy. The new tool is a frequency-switched CO₂ laser. A highly stable laser design was modified to include an intra cavity electro-optic modulator, which al lows the output of the laser to be frequency-switched. The frequency modulated output is used in spectroscopic experiments whose goals are the determination of decay rates for infrared moIecuIar transitions. The use of a frequency-switched laser is the most prom i sing means of making such measurements on nonpoIar molecules. The use of an electro-optic crystal inside a laser cavity introduces a number of fundamental problems which must be overcome before the instrument can be used to make useful spectroscopic measurements. These problems are brought about by the need for a stable laser amplitude and frequency output. The development of a novel stabilization technique to overcome these problems is documented in this thesis. Also included in this thesis is a description of the microcomputer and associated electronics necessary to integrate the laser into an experimental apparatus capable of performing signal averaging and background subtraction on raw time resolved data. The final chapters of this work describe experiments and results of measurements of the scattering cross sect ions of a nonpolar molecule with rare gas perturbers. The nonpolar molecule is SF₆ and the rare gas collision partners are Helium, Argon, and Xenon. The results indicate that the scattering cross section for state changing collisions displays a mass dependance predicted by classical collision theory. However, the measured cross sections for elastic velocity-changing collisions appears to be mass independent, which is at variance with theory.