In a recent Letter by Pakoulev et al. [CPL 371 (2003) 594], time-resolved anti-Stokes Raman measurements of the spectral evolution and relaxation of the OH stretch vibrations of pure H2O were presented. These measurements led the authors to reinterpret the results of previous femtosecond mid-infrared pump-probe studies on water. Here we show that this reinterpretation is incorrect.

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Journal Chem. Phys. Lett.
Bakker, H.J, Lock, A.J, & Madsen, D. (2004). Comment on: Vibrational relaxation and spectral evoluton following ultrafast OH stretch excitation of water by A.Pakoulev, Z. Wang, D.D. Dlott. Chem. Phys. Lett., 385, 329–331. doi:10.1016/j.cplett.2003.12.079