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J. Phys. Chem. Lett. In The Journal of Physical Chemistry Letters (2 October 2012), pp. 3001-3006, doi:10.1021/jz3012723 Key: citeulike:11397379
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Since the basal plane surface of ice was first observed by sum frequency generation, an extraordinarily intense band for the hydrogen(H)-bonded OH stretching vibration has been a matter of debate. We elucidate the remarkable spectral feature of the ice surface by quantum mechanics/molecular mechanics calculations. The intense H-bonded band is originated mostly from the ?bilayer-stitching? modes of a few surface bilayers, through significant intermolecular charge transfer. The mechanism of enhanced signal is sensitive to the order of the tetrahedral ice structure, as the charge transfer is coupled to the vibrational delocalization.
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