- Vibrational response of hydrogen-bonded interfacial water is dominated by intramolecular coupling
- Physical Review Letters
- Volume | Issue number
- 100 | 17
- Number of pages
- Document type
- Faculty of Science (FNWI)
- Swammerdam Institute for Life Sciences (SILS)
Van 't Hoff Institute for Molecular Sciences (HIMS)
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.
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