Bulk-like Vibrational Coupling of Surface Water Revealed by Sum-Frequency Generation Spectroscopy

16 December 2022, Version 1
This content is a preprint and has not undergone peer review at the time of posting.


Vibrational coupling between interfacial water molecules is important for energy dissipation after on-water chemistry, yet intensely debated. Here, we quantify the interfacial vibrational coupling strength through the linewidth of surface-specific vibrational spectra of the water’s O-H (O-D) stretch region for neat H2O/D2O and their isotopic mixtures. The local-field-effect-corrected experimental SFG spectra reveal that the vibrational coupling between hydrogen-bonded interfacial water O-H groups is very similar to that in bulk water, despite the effective density reduction at the interface.


Water Surface
SFG spectroscopy
Fresnel factor correction
isotopic dilution
vibrational coupling


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