Dynamics and vibrational coupling of methyl acetate dissolved in ethanol

•Two distinct vibrational bands have been assigned to two different types of MA molecules.•Physical properties exhibit a change below and above ∼0.6 vol fraction of MA.•Microviscosity model fails to predict dephasing times for higher ethanol concentrations.•NCE is due to repulsive interactions and is related to the vibrational relaxation process.•Onsager–Fröhlich dielectric model provides a fair agreement with the NCE results.