title: Three-dimensional infrared spectroscopy of isotope-substituted liquid water reveals heterogeneous dynamics.
abstract: 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.
authors.affiliation: Institute of Physical Chemistry, University of Zurich, Zurich, Switzerland.
authors.forename: Sean
authors.initials: S
authors.lastname: Garrett-Roe
authors.forename: Fivos
authors.initials: F
authors.lastname: Perakis
authors.forename: Francesco
authors.initials: F
authors.lastname: Rao
authors.forename: Peter
authors.initials: P
authors.lastname: Hamm