Abstract
Abstract The analysis of the rotational sub-band structure in the B bandsystem of methyl iodide by Mulliken and Teller has been extended to all four states of the …4 a 1 2 2 e 3 6 sa 1 Rydberg (R6 s ) configuration. All available one- and two-photon absorption data can be reproduced using a single set of molecular constants and selection rules derived by generalizing the frame transformation of the quantum defect theory to a symmetric top molecule. It is shown that electronic—nuclear interactions in addition to the electronic Coriolis coupling term must be included in an interpretation of the rotational structure of the R6 s states. In particular, uncoupling of the spin of the Rydberg electron from the molecular axis is a key element in understanding the results. Molecular constants obtained by fitting experimental bandshapes of the R6 s origins are shown to be those of the alternative levels of the freely-rotating, electronically-degenerate molecular ion core, CH 3 I + ( 2 E 3 2 , 1 2 ).
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