Ultrafast Vibrational Dynamics at Water Interfaces

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Science  29 Sep 2006:
Vol. 313, Issue 5795, pp. 1945-1948
DOI: 10.1126/science.1131536

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Time-resolved sum-frequency vibrational spectroscopy permits the study of hitherto neglected ultrafast vibrational dynamics of neat water interfaces. Measurements on interfacial bonded OH stretch modes revealed relaxation behavior on sub-picosecond time scales in close resemblance to that of bulk water. Vibrational excitation is followed by spectral diffusion, vibrational relaxation, and thermalization in the hydrogen-bonding network. Dephasing of the excitation occurs in ≤100 femtoseconds. Population relaxation of the dangling OH stretch was found to have a time constant of 1.3 picoseconds, the same as that for excitation transfer between hydrogen-bonded and unbonded OH stretches of water molecules surrounded by acetone.

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