Dresden 2011 – scientific programme
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MO: Fachverband Molekülphysik
MO 9: Femtosecond Spectroscopy II
MO 9.4: Talk
Tuesday, March 15, 2011, 11:30–11:45, TOE 317
Ultrafast Structural Dynamics in Hydrogen-Bonded Liquids from Coherent Multidimensional Infrared Spectroscopy of Vibrational Excitons — •Alexander Paarmann1,2 and R. J. Dwayne Miller1,3 — 1Departments of Chemistry and Physics, University of Toronto, Canada — 2Fritz-Haber Institute of the MPG, Berlin, Germany — 3Max Planck Research Group for Atomically Resolved Dynamics, Department of Physics, University of Hamburg, the Centre for Free Electron Laser Science/DESY, Germany
Coherent two-dimensional infrared (2DIR) spectroscopy is a powerful new method to study temporal as well as spatial correlations in hydrogen-bond networks. We present experimental and theoretical studies of the 2DIR response of two hydrogen-bonded liquids: water and formamide. For liquid water, temperature dependence of the 2DIR spectra revealed strong spatial correlations close to the freezing point, where the OH-stretching vibrations show significant spatial delocalization [1]. The 2DIR response from the more structured formamide exhibits a quite different behavior, being sensitive to time-averaged dipole arrangements and vibrational energy transfer dynamics within the H-bond network. These results are supported by theoretical calculations of the 2DIR spectra [2].
[1] D. Kraemer,M. L. Cowan, A. Paarmann, N. Huse, E. T. J. Nibbering, T. Elsaesser, and R. J. Dwayne Miller, Proc. Natl. Acad. Sci. USA 2008 105: 437-442
[2] A. Paarmann, T. Hayashi, S. Mukamel, R. J. D. Miller, J. Chem. Phys. 2008 128: 191103