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

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  • Sietse T. van der Post

    (FOM Institute AMOLF)

  • Cho-Shuen Hsieh

    (FOM Institute AMOLF
    Max-Planck Institute for Polymer Research
    Present address: Center for Molecular Spectroscopy and Dynamics, Institute for Basic Science (IBS), Seoul 136-701, Korea)

  • Masanari Okuno

    (Max-Planck Institute for Polymer Research
    Present address: Division of Chemistry, Graduate School of Pure and Applied Sciences, University of Tsukuba, Tennodai, Tsukuba, 305-8571, Japan)

  • 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)

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.

Suggested Citation

  • Sietse T. van der Post & Cho-Shuen Hsieh & Masanari Okuno & Yuki Nagata & Huib J. Bakker & Mischa Bonn & Johannes Hunger, 2015. "Strong frequency dependence of vibrational relaxation in bulk and surface water reveals sub-picosecond structural heterogeneity," Nature Communications, Nature, vol. 6(1), pages 1-7, December.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms9384
    DOI: 10.1038/ncomms9384
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    Cited by:

    1. Woongmo Sung & Ken-ichi Inoue & Satoshi Nihonyanagi & Tahei Tahara, 2024. "Unified picture of vibrational relaxation of OH stretch at the air/water interface," Nature Communications, Nature, vol. 15(1), pages 1-11, December.

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