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Interface-specific hydrogen- (H-)bonding network of water next to a substrate(including air) directly controls the energy transfer and chemical reactionpathway at many charged aqueous interfaces. Yet, experimental characterizationof such bonded water layer structure is still a challenge due to the presenceof the ion diffuse layer. We now develop a sum-frequency (SF) spectroscopicscheme with varying photon momentums as an all-optic solution for retrievingthe vibrational spectra of the bonded water layer and the diffuse layer, andhence microscopic structural and charging information about an interface.Application of the method to a charged surfactant-water interface reveals ahidden weakly-donor-H-bonded water species, suggesting an asymmetrichydration-shell structure of fully solvated surfactant headgroups. In anotherapplication to a zwitterionic phosphatidylcholine (PC) lipid monolayer-waterinterface, we find a highly polarized bonded water layer structure associatingto the PC headgroup, while the diffuse layer contribution is experimentallyproven to be negligible. Our all-optic method offers not only an in situmicroscopic probe of the electrochemical and biological interfaces, but also anew opportunity for promoting these researches toward high spatial and temporalresolutions.

Momentum-Resolved Sum-Frequency Vibrational Spectroscopy of Bonded Interface Layer at Charged Water Interfaces