Three-Dimensional Infrared Spectroscopy of Isotope-Substituted Liquid Water Reveals Heterogeneous Dynamics

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• 作者：Sean Garrett-Roe ; Fivos Perakis ; Francesco Rao ; Peter Hamm
• 刊名：Journal of Physical Chemistry B
• 出版年：2011
• 出版时间：June 2, 2011
• 年：2011
• 卷：115
• 期：21
• 页码：6976-6984
• 全文大小：962K
• 年卷期：v.115,no.21(June 2, 2011)
• ISSN：1520-5207

文摘

The dynamics of the hydrogen bond network of isotopically substituted liquid water are investigated with a new ultrafast nonlinear vibrational spectroscopy, three-dimensional infrared spectroscopy (3D-IR). The 3D-IR spectroscopy is sensitive to three-point frequency fluctuation correlation functions, and the measurements reveal heterogeneous structural relaxation dynamics. We interpret these results as subensembles of water which do not interconvert on a half picosecond time scale. We connect the experimental results to molecular dynamics (MD) simulations, performing a line shape analysis as well as complex network analysis.