期刊
JOURNAL OF CHEMICAL PHYSICS
卷 139, 期 16, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4826095
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资金
- Japan Society for the Promotion of Science (JSPS) [24245006, 25288014]
- Grants-in-Aid for Scientific Research [25288014] Funding Source: KAKEN
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. (C) 2013 AIP Publishing LLC.
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