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Knowledge of the interfacial water structure is essential for a basic understanding of the many environmental, technological, and biophysical systems in which aqueous interfaces appear. Using ultrafast two-dimensional surface-specific vibrational spectroscopy we show that the structure of heavy water at the water-air interface displays short-lived heterogeneity and is very different from that at the water-lipid interfac

Communication: Interfacial water structure revealed by ultrafast two-dimensional surface vibrational spectroscopy