A first principles molecular dynamics study of vibrational spectral diffusion and hydrogen bond dynamics in liquid methanol

► An ab initio simulation study is performed on deuterated liquid methanol at room temperature. ► The frequency-structure correlations of methanol molecules are investigated. ► Calculations are made for dynamics of hydrogen bonds and frequency fluctuations. ► Vibrational spectral hole dynamics calculations are also performed for selected OD stretch modes. ► The correlations of hydrogen bond relaxation with vibrational frequency fluctuations are discussed.