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Coupling between intra- and intermolecular motions in liquid water revealed by two-dimensional terahertz-infrared-visible spectroscopy

Author

Listed:
  • Maksim Grechko

    (Max Planck Institute for Polymer Research)

  • Taisuke Hasegawa

    (Max Planck Institute for Polymer Research)

  • Francesco D’Angelo

    (Max Planck Institute for Polymer Research)

  • Hironobu Ito

    (Shizuoka University)

  • Dmitry Turchinovich

    (Max Planck Institute for Polymer Research
    Universität Duisburg-Essen)

  • Yuki Nagata

    (Max Planck Institute for Polymer Research)

  • Mischa Bonn

    (Max Planck Institute for Polymer Research)

Abstract

The interaction between intramolecular and intermolecular degrees of freedom in liquid water underlies fundamental chemical and physical phenomena such as energy dissipation and proton transfer. Yet, it has been challenging to elucidate the coupling between these different types of modes. Here, we report on the direct observation and quantification of the coupling between intermolecular and intramolecular coordinates using two-dimensional, ultra-broadband, terahertz-infrared-visible (2D TIRV) spectroscopy and molecular dynamics calculations. Our study reveals strong coupling of the O-H stretch vibration, independent of the degree of delocalization of this high-frequency mode, to low-frequency intermolecular motions over a wide frequency range from 50 to 250 cm−1, corresponding to both the intermolecular hydrogen bond bending (≈ 60 cm−1) and stretching (≈ 180 cm−1) modes. Our results provide mechanistic insights into the coupling of the O-H stretch vibration to collective, delocalized intermolecular modes.

Suggested Citation

  • Maksim Grechko & Taisuke Hasegawa & Francesco D’Angelo & Hironobu Ito & Dmitry Turchinovich & Yuki Nagata & Mischa Bonn, 2018. "Coupling between intra- and intermolecular motions in liquid water revealed by two-dimensional terahertz-infrared-visible spectroscopy," Nature Communications, Nature, vol. 9(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:9:y:2018:i:1:d:10.1038_s41467-018-03303-y
    DOI: 10.1038/s41467-018-03303-y
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    Cited by:

    1. Danhua Dai & Xianwei Wang & Yiwei Liu & Xiao-Liang Yang & Clemens Glaubitz & Vasyl Denysenkov & Xiao He & Thomas Prisner & Jiafei Mao, 2021. "Room-temperature dynamic nuclear polarization enhanced NMR spectroscopy of small biological molecules in water," Nature Communications, Nature, vol. 12(1), pages 1-15, December.
    2. Tomislav Begušić & Geoffrey A. Blake, 2023. "Two-dimensional infrared-Raman spectroscopy as a probe of water’s tetrahedrality," Nature Communications, Nature, vol. 14(1), pages 1-10, December.

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