Abstract
We report a femtosecond time-resolved study of water at the neat water-air interface. The O-H stretch vibrational lifetime of hydrogen-bonded interfacial water is measured using surface-specific 4th-order nonlinear optical spectroscopy with femtosecond infrared pulses. The vibrational lifetime in the frequency range of 3200 to 3500 cm(-1) is found to closely resemble that of bulk water, indicating ultrafast exchange of vibrational energy between surface water molecules and those in the bulk.
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