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Here we report a detailed study on spectroscopy, structure and dynamics ofwater molecules at air/water interface, investigated with Sum FrequencyGeneration Vibrational Spectroscopy (SFG-VS). Quantitative polarization andexperimental configuration analysis of the SFG data in different polarizationswith four sets of experimental configurations can shed new lights on ourpresent understanding of the air/water interface. Firstly, we concluded thatthe motion of the interfacial water molecules can only be in a limited angularrange, instead rapidly varying over a broad angular range in the vibrationalrelaxation time suggested previously. Secondly, because different vibrationalmodes of different molecular species at the interface has different symmetryproperties, polarization and symmetry analysis of the SFG-VS spectral featurescan help assignment of the SFG-VS spectra peaks to different interfacialspecies. These analysis concluded that the narrow 3693cm-1 and broad 3550cm-1peaks belong to C_ v symmetry, while the broad 3250cm-1 and 3450cm-1 peaksbelong to the symmetric stretching modes with C_2v symmetry. Thus, the 3693cm-1peak is assigned to the free OH, the 3550cm-1 peak is assigned to the singlehydrogen bonded OH stretching mode, and the 3250cm-1 and 3450cm-1 peaks areassigned to interfacial water molecules as two hydrogen donors for hydrogenbonding (with C_2v symmetry), respectively. Thirdly, analysis of the SFG-VSspectra concluded that the singly hydrogen bonded water molecules at theair/water interface have their dipole vector direct almost parallel to theinterface, and is with a very narrow orientational distribution. The doublyhydrogen bond donor water molecules have their dipole vector point away fromthe liquid phase

journal of chemical physics online/the journal of chemical physics/journal of chemical physics

Polarization and experimental configuration analyses of sum frequency generation vibrational spectra, structure, and orientational motion of the air/water interface