Three-dimensional infrared spectroscopy of isotope-substituted liquid water reveals heterogeneous dynamics.

نویسندگان

  • Sean Garrett-Roe
  • Fivos Perakis
  • Francesco Rao
  • Peter Hamm
چکیده

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.

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عنوان ژورنال:
  • The journal of physical chemistry. B

دوره 115 21  شماره 

صفحات  -

تاریخ انتشار 2011