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Energy transfer within the hydrogen bonding network of water following resonant terahertz excitation

MPS-Authors
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Kampfrath,  Tobias
Physical Chemistry, Fritz Haber Institute, Max Planck Society;
Department of Physics, Freie Universität Berlin;

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Balos,  Vasileios
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Wolf,  Martin
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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Sajadi,  Mohsen
Physical Chemistry, Fritz Haber Institute, Max Planck Society;

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2003.08651.pdf
(Preprint), 2MB

eaay7074.full.pdf
(Publisher version), 1021KB

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Citation

Elgabarty, H., Kampfrath, T., Bonthuis, D. J., Balos, V., Kaliannan, N. K., Loche, P., et al. (2020). Energy transfer within the hydrogen bonding network of water following resonant terahertz excitation. Science Advances, 6(17): eaay7074. doi:10.1126/sciadv.aay7074.


Cite as: http://hdl.handle.net/21.11116/0000-0005-F951-7
Abstract
Energy dissipation in water is very fast and more efficient than in many other liquids. This behavior is commonly attributed to the intermolecular interactions associated with hydrogen bonding. Here, we investigate the dynamic energy flow in the hydrogen-bond network of liquid water by a pump-probe experiment. We resonantly excite intermolecular degrees of freedom with ultrashort single-cycle terahertz pulses and monitor its Raman response. By using ultrathin sample-cell windows, a background-free bipolar signal whose tail relaxes mono-exponentially is obtained. The relaxation is attributed to the molecular translational motions, using complementary experiments, force-field and ab initio molecular dynamics simulations. They reveal an initial coupling of the terahertz electric field to the molecular rotational degrees of freedom whose energy is rapidly transferred, within the excitation pulse duration, to the restricted-translational motion of neighboring molecules. This rapid energy transfer may be rationalized by the strong anharmonicity of the intermolecular interactions.