title: Origin of Vibrational Spectroscopic Response at Ice Surface.
abstract: 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.
authors: Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan.
authors: Tatsuya
authors: T
authors: Ishiyama
authors: Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan.
authors: Hideaki
authors: H
authors: Takahashi
authors: Department of Chemistry, Graduate School of Science, Tohoku University, Sendai 980-8578, Japan.
authors: Akihiro
authors: A
authors: Morita
keywords: charge transfer; hydrogen bonding network; molecular dynamics; sum frequency generation; vibrational delocalization