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The influence of dimethyl sulfoxide (DMSO) on the hydration of a peptide group has been explored by measuring the FTIR spectrum of N-methylacetamide in different mixtures of DMSO and D2O. An analysis of the amide I’ profile indicates two processes. For DMSO mole fractions between 0 and 0.5, the hydration shell on the side of the carbonyl group is systematically perturbed, which leads to a destabilization...