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Water and alcohols show characteristic properties due to the formation of hydrogen-bonding networks in the liquid or in the solution state. They are classified as a group of structural liquids.12 Recently, the structure of water-alcohol solutions over the whole composition region has been extensively studied by X-ray diffraction3, NMR4, mass spectrometry5'6, dielectric measurements7'8, and thermodynamic calculations.9, to These studies have focused on the change in the cluster structure formed by water and alcohol molecules as the composition of the solutions varies. We reported an observation which suggested such structural changes by a high-frequency dielectric technique.11 With this technique we studied in detail the dielectric behavior of solutions with respect to the composition change, and found that it was sensitive to small changes in the dielectric behavior. In this letter we report on some observations of stepwise changes in the resonance frequency, suggesting a structural phase transition for water solutions of four kinds of alcohols, methanol, ethanol, 1-propanol, and 2-propanol.

Stepwise Change in the Resonance Frequency of Water-Alcohol Mixtures, Suggesting a Rearrangement of the Solution Structure