The coherent Raman emission from primary alcohols [CH3(CH2)nOH, n = 0–10], 2-propyl alcohol and tert-butyl alcohol was studied using a frequency-doubled Nd :YAG pump laser (532 nm). We show that increases in the chain length (CH2 groups) and the number of CH3 groups in the alcohols (CH3 > CH2) enhance the Raman emission efficiency. Theoretical density functional theory (DFT) calculations and frequency scaling allow one to associate the vibrational wavenumbers with the molecular fragment responsible for the vibration. We obtained good agreement between the observed phenomena and the predictions of the theoryFONACIT(Grant G97000593).