Strong frequency dependence of vibrational relaxation in bulk and surface water reveals sub-picosecond structural heterogeneity

Sietse T. van der Post, Cho-Shuen Hsieh, Masanari Okuno, Yuki Nagata, Huib J. Bakker (), Mischa Bonn () and Johannes Hunger
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Sietse T. van der Post: FOM Institute AMOLF
Cho-Shuen Hsieh: FOM Institute AMOLF
Masanari Okuno: Max-Planck Institute for Polymer Research
Yuki Nagata: Max-Planck Institute for Polymer Research
Huib J. Bakker: FOM Institute AMOLF
Mischa Bonn: Max-Planck Institute for Polymer Research
Johannes Hunger: Max-Planck Institute for Polymer Research

Nature Communications, 2015, vol. 6, issue 1, 1-7

Abstract: Abstract Because of strong hydrogen bonding in liquid water, intermolecular interactions between water molecules are highly delocalized. Previous two-dimensional infrared spectroscopy experiments have indicated that this delocalization smears out the structural heterogeneity of neat H2O. Here we report on a systematic investigation of the ultrafast vibrational relaxation of bulk and interfacial water using time-resolved infrared and sum-frequency generation spectroscopies. These experiments reveal a remarkably strong dependence of the vibrational relaxation time on the frequency of the OH stretching vibration of liquid water in the bulk and at the air/water interface. For bulk water, the vibrational relaxation time increases continuously from 250 to 550 fs when the frequency is increased from 3,100 to 3,700 cm−1. For hydrogen-bonded water at the air/water interface, the frequency dependence is even stronger. These results directly demonstrate that liquid water possesses substantial structural heterogeneity, both in the bulk and at the surface.

Date: 2015
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DOI: 10.1038/ncomms9384

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