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Journal of Physical Chemistry A, Vol.111, No.5, 743-746, 2007
Ultrafast structural dynamics of water induced by dissipation of vibrational energy
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 similar to 1 ps time scale and is connected with the breaking of hydrogen bonds, resulting in a macroscopically heated liquid.