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Ultrafast Structural Dynamics of Water Induced by Dissipation of Vibrational Energy

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    Ultrafast Structural Dynamics of Water Induced by Dissipation of Vibrational Energy
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    Max Born Institut für Nichtlineare Optik und Kurzzeitspektroskopie, 12489 Berlin, Germany, and Institute of Industrial Science, University of Tokyo, Tokyo 153-8505, Japan
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    The Journal of Physical Chemistry A

    Cite this: J. Phys. Chem. A 2007, 111, 5, 743–746
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    https://doi.org/10.1021/jp0676538
    Published January 11, 2007
    Copyright © 2007 American Chemical Society
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    Abstract

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    In the liquid phase, water molecules form a disordered fluctuating network of intermolecular hydrogen bonds. Using both inter- and intramolecular vibrations as structural probes in ultrafast infrared spectroscopy, we demonstrate a two-stage structural response of this network to energy disposal:  vibrational energy from individually excited water molecules is transferred to intermolecular modes, resulting in a sub-100 fs nuclear rearrangement that leaves the local hydrogen bonds weakened but unbroken. Subsequent energy delocalization over many molecules occurs on an ∼1 ps time scale and is connected with the breaking of hydrogen bonds, resulting in a macroscopically heated liquid.

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    †

     Max Born Institut für Nichtlineare Optik und Kurzzeitspektroskopie.

    ‡

     University of Tokyo.

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     To whom correspondence should be addressed. Phone:  +49 30 6392 1400. Fax:  +49 30 6392 1409. E-mail:  [email protected].

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    Cite this: J. Phys. Chem. A 2007, 111, 5, 743–746
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    https://doi.org/10.1021/jp0676538
    Published January 11, 2007
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