Abstract
A combination of vibrational spectroscopy and molecular calculations reveals that only the surface layer of water at the interface with air has a distinctly different structure from the bulk liquid. See Letter p.192 Surface phenomena at the air–water interface are of vital importance in many situations, from oceanography to atmospheric and environmental chemistry. An unanswered question in the field is how thin is the interfacial region — or how soon do the properties of bulk liquid water reappear as the interface is crossed. Using spectroscopy to probe the 'free OD' vibrational mode of water molecules with an oxygen–deuterium bond protruding from the surface and theoretical modelling to interpret the results, Stiopkin et al. find that water molecules straddling the interface form hydrogen bonds that are only slightly weaker than those in bulk water. This suggests a remarkably rapid onset of bulk-phase behaviour, and an extremely short 'healing length' for the interface on crossing from the air into the water phase.
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