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We will explore a variant of resonant two-photon ionization (R2PI). Development of the IR + UV R2PI experiment is underway. We have used optical R2PI and pulsed field ionization detection to obtain vibrational spectra of the benzyl and phenylsilane cations. In benzyl, we have learned about the vibronic coupling in the mixed 1[sup 2]A[sub 2]-2[sup 2]B[sub 2] system near 450 nm by projecting the mixed states onto the manifold of cation vibrational states. In phenylsilane[sup +], we find that the sixfold barrier to internal rotation of the silyl group is small (V[sub 6]= +19 cm[sup [minus]1]). We are beginning to understand the mechanisms of coupling of torsional states with vibrations, overall rotation, and other electronic states, and we are developing a model of internal rotation in aromatic compounds based on Weinhold's natural resonance theory. 1 tab, 14 refs.

Infrared spectroscopy of organic free radicals related to combustion processes