The stimulated Raman spectrum of water and its relationship to liquid structure

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Abstract
Stimulated Raman spectra (SRS) of H2O, D2O, H2O–D2O mixtures, and aqueous solutions of NaClO4 have been measured using a mode‐locked, stabilized Nd glass laser operating in the TEM00 mode. Spectra with relatively narrow peaks were obtained in all cases, as predicted by the first order theory of SRS. Other effects (such as multiple peaks, broadened spectra, and shifted peaks), which have been interpreted as evidence for a mixture model of water, are reconsidered, and it is argued that they are either artifacts arising from modulation by stimulation in the hydrogen bond bending region or arise from disruption of thermal equilibrium in filaments due to the high electric fields present in the focused laser beam.