![]() We thus formulate a new definition for capturing the subensemble of the surface free O-H groups using the intermolecular distance and the angle formed by the water dimer, through the comparison of the ∼3700 cm -1 SFG response and the responses from the selected free O-H groups at the HOD-air interface. Our data show that commonly used hydrogen bond definitions do not adequately capture the free O-H groups contributing to the 3700 cm -1 peak. ![]() Although these free O-H groups are often defined as the O-H groups which are not hydrogen-bonded to other water molecules, a direct correlation between such non-hydrogen-bonded O-H groups and the 3700 cm -1 SFG response has been lacking. In surface-specific vibrational spectroscopic studies using sum-frequency generation (SFG) spectroscopy, free O-H groups are experimentally well characterized in the O-H stretch region by a sharp 3700 cm -1 peak. for water contact with hydrophobic protein residues, or at the water-air interface. ![]() Free O-H groups of water are often found at the water-hydrophobic medium interface, e.g. ![]()
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