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Previous vibrational assignments for Me4N+ are examined and in some respects revised. Frequency and intensity changes in the Raman spectra of Me,NCI solutions with variations of concentration and solvent (D20 and CD,OH) were observed mainly in the CH stretching and NC4 bending regions. These are interpreted in terms of cation-anion associations the extent of which is found to be much larger in methanolic than in aqueous solution. The effects of temperature on the Raman bands proved to be much smaller than those of concentration or solvent changes.

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