Origin of Vibrational Spectroscopic Response at Ice Surface
详细信息 查看全文
- 作者：Tatsuya Ishiyama ; Hideaki Takahashi ; Akihiro Morita
- 刊名：The Journal of Physical Chemistry Letters
- 出版年：2012
- 出版时间：October 18, 2012
- 年：2012
- 卷：3
- 期：20
- 页码：3001-3006
- 全文大小：403K
- 年卷期：v.3,no.20(October 18, 2012)
- ISSN：1948-7185
文摘
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 鈥渂ilayer-stitching鈥?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.