Isotopic Dilution Study of the Water/Vapor Interface by Phase-Sensitive Sum-Frequency Vibrational Spectroscopy

Phase-sensitive sum-frequency vibrational spectroscopy (PS-SFVS) has been used to probe the isotopically diluted water/vapor interfaces in the spectral regions of OD (2200−2800 cm−1) and OH (3000−3800 cm−1) stretches. The experimentally measured Im χ S (2) spectra, where χ S (2) is the surface nonli...

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Published inJournal of the American Chemical Society Vol. 131; no. 8; pp. 2790 - 2791
Main Authors Tian, Chuan-Shan, Shen, Y. Ron
Format Journal Article
LanguageEnglish
Published United States American Chemical Society 04.03.2009
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Summary:Phase-sensitive sum-frequency vibrational spectroscopy (PS-SFVS) has been used to probe the isotopically diluted water/vapor interfaces in the spectral regions of OD (2200−2800 cm−1) and OH (3000−3800 cm−1) stretches. The experimentally measured Im χ S (2) spectra, where χ S (2) is the surface nonlinear susceptibility, permit direct characterization of resonances of the interfaces. The Im χ S (2) spectrum of the HDO/vapor interface that is intrinsically simpler to analyze can be deduced from the result of isotopic dilution. It exhibits in the bonded-OH region a broad band comprising two parts with opposite signs, in contrast to those deduced earlier from fitting of the |χ S (2)|2 spectra and those calculated by MD simulation, but consistent with that obtained for the H2O/vapor interface.
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ISSN:0002-7863
1520-5126
DOI:10.1021/ja809497y