IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v15y2024i1d10.1038_s41467-024-45388-8.html
   My bibliography  Save this article

Unified picture of vibrational relaxation of OH stretch at the air/water interface

Author

Listed:
  • Woongmo Sung

    (RIKEN)

  • Ken-ichi Inoue

    (RIKEN
    Tohoku University)

  • Satoshi Nihonyanagi

    (RIKEN
    RIKEN Center for Advanced Photonics (RAP))

  • Tahei Tahara

    (RIKEN
    RIKEN Center for Advanced Photonics (RAP))

Abstract

The elucidation of the energy dissipation process is crucial for understanding various phenomena occurring in nature. Yet, the vibrational relaxation and its timescale at the water interface, where the hydrogen-bonding network is truncated, are not well understood and are still under debate. In the present study, we focus on the OH stretch of interfacial water at the air/water interface and investigate its vibrational relaxation by femtosecond time-resolved, heterodyne-detected vibrational sum-frequency generation (TR-HD-VSFG) spectroscopy. The temporal change of the vibrationally excited hydrogen-bonded (HB) OH stretch band (ν=1→2 transition) is measured, enabling us to determine reliable vibrational relaxation (T1) time. The T1 times obtained with direct excitations of HB OH stretch are 0.2-0.4 ps, which are similar to the T1 time in bulk water and do not noticeably change with the excitation frequency. It suggests that vibrational relaxation of the interfacial HB OH proceeds predominantly with the intramolecular relaxation mechanism as in the case of bulk water. The delayed rise and following decay of the excited-state HB OH band are observed with excitation of free OH stretch, indicating conversion from excited free OH to excited HB OH (~0.9 ps) followed by relaxation to low-frequency vibrations (~0.3 ps). This study provides a complete set of the T1 time of the interfacial OH stretch and presents a unified picture of its vibrational relaxation at the air/water interface.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45388-8
    DOI: 10.1038/s41467-024-45388-8
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-024-45388-8
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-024-45388-8?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    1. 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.
    2. Igor V. Stiopkin & Champika Weeraman & Piotr A. Pieniazek & Fadel Y. Shalhout & James L. Skinner & Alexander V. Benderskii, 2011. "Hydrogen bonding at the water surface revealed by isotopic dilution spectroscopy," Nature, Nature, vol. 474(7350), pages 192-195, June.
    3. Ken-ichi Inoue & Mohammed Ahmed & Satoshi Nihonyanagi & Tahei Tahara, 2020. "Reorientation-induced relaxation of free OH at the air/water interface revealed by ultrafast heterodyne-detected nonlinear spectroscopy," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    4. M. L. Cowan & B. D. Bruner & N. Huse & J. R. Dwyer & B. Chugh & E. T. J. Nibbering & T. Elsaesser & R. J. D. Miller, 2005. "Ultrafast memory loss and energy redistribution in the hydrogen bond network of liquid H2O," Nature, Nature, vol. 434(7030), pages 199-202, March.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Ulrich Bangert & Frank Stienkemeier & Lukas Bruder, 2022. "High-resolution two-dimensional electronic spectroscopy reveals the homogeneous line profile of chromophores solvated in nanoclusters," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    2. Heinz Langhals, 2017. "Interaction of Components in Molecular Optoelectronics for the Next Generation of IT Devices," Scientific Review, Academic Research Publishing Group, vol. 3(3), pages 17-28, 03-2017.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-45388-8. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.