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Infrared (IR) spectroscopy for N,N-dimethylformamide (DMF) shows that the OCN bend (δOCN) and the CO stretch (νCO) vibrations undergo an upshift and a downshift, respectively, on the dissolution of CClO4)2. Quantum chemical calculations are performed for optimizing the structures and predicting the IR spectra of model complexes for solute species. The calculations reveal that Co2+ exerts a much larger influence than ClO4- on the vibrations of DMF. For Co2+(DMF)6, in which each DMF molecule is coordinated to Co2+ via the O atom, the Co
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