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Stimulated Raman scattering (SRS) and spontaneous Raman spectra are both used here to study the hydrogen bond (H structure and kinetics of methanol (MeOH)-water mixtures in different volume ratios. We have found that when the volume fraction of MeOH ranges from 0 to 0.27, the HB structure of water molecules is enhanced, originating from the cooperation of the hydroxyl-enhanced HBs in liquid water and the formation of an ice-like structure around the methyl groups. However, when the volume fraction of MeOH goes beyond 0.27, the main