Since the first MD calculation of SFG spectrum of liquid water was reported by us in 2000, understandings of the water surface and its SFG spectroscopy have been greatly advanced.  In this talk, we summarize our recent efforts on the molecular dynamics analysis of interfacial water in collaboration with experiment.Systematic isotope dilution in combination with the phase-sensitive heterodyne detection of chi(2) were experimentally performed, and theresults were critically compared with recent MD simulation.  It was found that the MD result shows excellent agreement with the phase-sensitive experiment when the intra- and intermolecular vibrational coupling are turned off. QM/MM calculations of SFG spectra confirmed that the positive imaginary part of chi(2) in the low-frequency region (~3000 cm-1) reflects anisotropic response of strongly hydrogen-bonding water pairs.

Unified view of surface nonlinear susceptibility chi(2) of liquid water studied by molecular dynamics and sum frequency generation spectroscopy

243rd National Meeting (2012)

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