UC Santa Barbara

Vibrational spectroscopy in the gas phase is a powerful analytical tool for probing the structure of polyatomic molecules in an isolated, non-perturbative environment.This dissertation describes the development of a novel experimental technique for nondestructively measuring the vibrational spectrum of single gas phase polyatomic molecules. This is believed to be the first report of such a result. The underlying theory relevant to this method, as well as the experimental infrastructure which was constructed to facilitate it, is discussed in detail. Spectra of single molecular ions of multiple species are presented and analyzed, illustrating the general capabilities of this technique. This powerful new analytical tool has important implications for chemical analysis and fundamental physical chemistry experiments, along with other applications which are highlighted.