Application of highly time-resolved coherent anti-Stokes Raman scattering to chemical dynamics

The first part of this dissertation reports the results of state-to-state dynamics experiments on the D + H;The second part of this dissertation describes a method for deconvoluting incompletely resolved CARS spectra to obtain population distributions. No particular form for the population distributions is assumed, the population of each quantum state is treated as an independent variable. This method of analysis is different from previous ones which assume a Boltzmann population distribution and thus are limited to analysis of CARS spectra taken under thermal equilibrium conditions. The method of analysis reported here has been developed to deconvolute CARS spectra of photofragments and chemical reaction products obtained in chemical dynamics experiments under non-equilibrium conditions. The deconvolution procedure has been incorporated into a computer code that is listed in an appendix. The application of that code to the deconvolution of CARS spectra obtained for samples at thermal equilibrium and not at thermal equilibrium is reported.