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Interference effects in the sum frequency generation spectra of thin organic films. II: Applications to different thin-film systems

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Title: Interference effects in the sum frequency generation spectra of thin organic films. II: Applications to different thin-film systems
Authors: Tong, Yujin1 Browse this author
Zhao, Yanbao2 Browse this author
Li, Na3 Browse this author
Ma, Yunsheng4 Browse this author
Osawa, Masatoshi5 Browse this author
Davies, Paul B. Browse this author
Ye, Shen7 Browse this author →KAKEN DB
Authors(alt): 仝, 玉进1
赵, 彦保2
李, 娜3
马, 运生4
大澤, 雅俊5
叶, 深7
Issue Date: 21-Jul-2010
Publisher: American Institute of Physics
Journal Title: Journal of Chemical Physics
Volume: 133
Issue: 3
Start Page: 034705
Publisher DOI: 10.1063/1.3428673
PMID: 20649348
Abstract: In this paper, the results of the modeling calculations carried out for predicting the interference effects expected in the sum frequency generation (SFG) spectra of a specific thin-layer system, described in the accompanying paper, are tested by comparing them with the experimental spectra obtained for a real thin-layer film comprising an organic monolayer/variable thickness dielectric layer/gold substrate. In this system, two contributions to the SFG spectra arise, a resonant contribution from the organic film and a nonresonant contribution from the gold substrate. The modeling calculations are in excellent agreement with the experimental spectra over a wide range of thicknesses and for different polarization combinations. The introduction of another resonant monolayer adjacent to the gold substrate and with the molecules having a reverse orientation has a significant affect on the spectral shapes which is predicted. If a dielectric substrate such as CaF2 is used instead of a gold substrate, only the spectral intensities vary with the film thickness but not the spectral shapes. The counterpropagating beam geometry will change both the thickness dependent spectral shapes and the intensity of different vibrational modes in comparison with a copropagating geometry. The influences of these experimental factors, i.e., the molecular orientational structure in the thin film, the nature of the substrate, and the selected incident beam geometry, on the experimental SFG spectra are quantitatively predicted by the calculations. The thickness effects on the signals from a SFG active monolayer contained in a thin liquid-layer cell of the type frequently used for in situ electrochemical measurements is also discussed. The modeling calculation is also valid for application to other thin-film systems comprising more than two resonant SFG active interfaces by appropriate choice of optical geometries and relevant optical properties.
Rights: Copyright 2010 American Institute of Physics. This article may be downloaded for personal use only. Any other use requires prior permission of the author and the American Institute of Physics. The following article appeared in J. Chem. Phys. 133, 034705 (2010) and may be found at
Type: article
Appears in Collections:触媒科学研究所 (Institute for Catalysis) > 雑誌発表論文等 (Peer-reviewed Journal Articles, etc)

Submitter: 叶 深

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