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The coupling of electronic and nuclear motions in the rovibronic levels of the lowest Rydberg states of methyl iodide is discussed in terms of a frame transformation between lab- and body- frame coordinate systems for an s Rydberg electron in the field of an electronically-degenerate, symmetric-top molecular ion core. It is shown that the r-dependence of exchange, spin-orbit, spin-rotation, and vibronic interactions, where r is the radial distance of the electron from the ion core, must be considered in order to provide a consistent analysis of the experimental data. Molecular constants, obtained by fitting one- and two-photon absorption spectra, show conclusively that the spin of the Rydberg electron is uncoupled from the molecular frame. Bandshape fitting reveals that the interaction between electronic and vibrational angular momenta leads to complete angular momentum quenching in some vibronic levels, in which it appears that the vibrating core "traps" the Rydberg electron. constants permit extrapolation of channel mixing across ionization thresholds in CH3I but not in HI. discussion of these events is sketched. The magnitudes of the B rotational A theoretical frame for the

Angular momentum coupling in molecular Rydberg states