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Phys Rev Lett. 2008 May 2;100(17):173901. Epub 2008 Apr 28.

Vibrational response of hydrogen-bonded interfacial water is dominated by intramolecular coupling.

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FOM Institute for Atomic and Molecular Physics, Kruislaan 407, 1098 SJ, Amsterdam, The Netherlands.


Using the surface-specific vibrational technique of vibrational sum-frequency generation, we reveal that the double-peaked structure in the vibrational spectrum of hydrogen-bonded interfacial water molecules originates from vibrational coupling between the stretch and bending overtone, rather than from structural effects. This is demonstrated by isotopic dilution experiments, which reveal a smooth transition from two peaks to one peak, as D2O is converted into HDO. Our results show that the water interface is structurally more homogeneous than previously thought.

[Indexed for MEDLINE]

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