The interaction of N,N-dimethyl formamide (DMF) and N,N-dimethyl acetamide (DMA) with methanol in solution mixtures was studied using Fourier transform infrared–attenuated total reflection (FT-IR/ATR) spectroscopy. The concentration-dependent FT-IR/ATR spectra of DMF/methanol and DMA/methanol mixtures were recorded in the wavenumber range 4000–650 cm<sup>–1</sup> to investigate wavenumber shifts as a consequence of hydrogen bonding interactions. In combination with two-dimensional correlation spectroscopy (2D-COS), the positional fluctuations observed in the ν(C=O) and ν(O–H) regions of DMF/DMA and methanol, respectively, have been discussed in terms of changing populations of differently hydrogen-bonded and interacting species of the same and different component molecules.
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