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Updated: May 6, 2026

Author Spotlight: Unveiling the Potential of VSFG Microscopy in Studying Mesoscopically Heterogeneous Self-Assembled Structures
Published on: December 1, 2023
Communication: Ultrafast vibrational dynamics of hydrogen bond network terminated at the air∕water interface: a
Prashant Chandra Singh1, Satoshi Nihonyanagi, Shoichi Yamaguchi
1Molecular Spectroscopy Laboratory, RIKEN, Wako, Saitama 351-0198, Japan.
Abstract:
Ultrafast vibrational dynamics of hydrogen bond network at the air∕water interface is revealed by two-dimensional heterodyne-detected vibrational sum frequency generation (2D HD-VSFG) spectroscopy. Three diagonal peaks are clearly observed in the 2D HD-VSFG spectrum, which correspond to the negative and positive hydrogen-bonded OH stretch bands and the positive "free" OH stretch band in the steady-state HD-VSFG spectrum. A diagonally elongated bleaching lobe of the hydrogen-bonded OH at 0 ps indicates that it is partly inhomogeneously broadened. This diagonal elongation vanishes in a few hundred femtoseconds, implying the ultrafast spectral diffusion in the hydrogen-bonded OH band. Off-diagonal cross peaks between each OH oscillator are clearly observed instantaneously within the time resolution of 0.2 ps, suggesting that they are vibrationally coupled through anharmonicity and∕or energy transfer.
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