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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
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    References listed on IDEAS

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    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.
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