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| - Spectral Interference and Molecular Conformation at Liquid Interface with Sum FrequencyGeneration Vibrational Spectroscopy (SFG-VS)
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| - In this report, we present an analysis of the interference effects in the SFG-VS spectra of the vapor/ethanolinterfaces with normal and deuterated liquid ethanol. Crucial information on the ethanol molecular orientationcan be obtained from analyzing the interference effects between the different SFG-VS spectral features. Withthe strength-coupled orientational functional dr(θ) of the different spectral features from the same or differentmolecular groups, and with the phase information contained in the SFG spectra measured under differentpolarization combinations, the detailed orientational conformation structure of the ethanol molecule at thevapor/ethanol interface can be obtained. The ethanol molecule is found to possess an orientational conformationwith its CH3- group pointing away from the liquid phase at an orientational tilt angle of about 45°, its -CH2-group away from the liquid interface around 10°, and the C−C−O plane is near perpendicular to the planeof interface. Here, the conclusion that the -CH2- group has to tilt away from the liquid phase can only bereached with the knowledge of the spectral overlap and the analysis of the interference between the overlappingspectral features. The details of the molecular orientation angle and the orientational distribution width werediscussed with novel approaches. These results suggested that studying coherent interference effects in thepolarization analysis in SFG-VS can provide novel understanding of the interfacial molecular structure andinteractions. The tools and the concepts of SFG-VS analysis developed in this study can be applied to morecomplex molecular interfaces and thin films.
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