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

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 f...

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Veröffentlicht in:Physical review letters 2008-05, Vol.100 (17), p.173901
Hauptverfasser: Sovago, Maria, Campen, R Kramer, Wurpel, George W H, Müller, Michiel, Bakker, Huib J, Bonn, Mischa
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Sprache:eng
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Zusammenfassung: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.
ISSN:0031-9007
DOI:10.1103/PhysRevLett.100.173901