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题名: Quantitative spectral and orientational analysis in surface sum frequency generation vibrational spectroscopy (SFG-VS)
作者: Wang, HF;  Gan, W;  Lu, R;  Rao, Y;  Wu, BH
刊名: INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY
发表日期: 2005-04-01
DOI: 10.1080/01442350500225894
卷: 24, 期:2, 页:191-256
收录类别: SCI
文章类型: Review
WOS标题词: Science & Technology ;  Physical Sciences
类目[WOS]: Chemistry, Physical ;  Physics, Atomic, Molecular & Chemical
研究领域[WOS]: Chemistry ;  Physics
英文摘要: Sum frequency generation vibrational spectroscopy (SFG-VS) has been proven to be a uniquely effective spectroscopic technique in the investigation of molecular structure and conformations, as well as the dynamics of molecular interfaces. However, the ability to apply SFG-VS to complex molecular interfaces has been limited by the ability to abstract quantitative information from SFG-VS experiments. In this review, we try to make assessments of the limitations, issues and techniques as well as methodologies in quantitative orientational and spectral analysis with SFG-VS. Based on these assessments, we also try to summarize recent developments in methodologies on quantitative orientational and spectral analysis in SFG-VS, and their applications to detailed analysis of SFG-VS data of various vapour/neat liquid interfaces. A rigorous formulation of the polarization null angle (PNA) method is given for accurate determination of the orientational parameter D = [cos theta]/[cos(3) theta], and comparison between the PNA method with the commonly used polarization intensity ratio (PIR) method is discussed. The polarization and incident angle dependencies of the SFG-VS intensity are also reviewed, in the light of how experimental arrangements can be optimized to effectively abstract crucial information from the SFG-VS experiments. The values and models of the local field factors in the molecular layers are discussed. In order to examine the validity and limitations of the bond polarizability derivative model, the general expressions for molecular hyperpolarizability tensors and their expression with the bond polarizability derivative model for C-3v, C-2v and C-infinity v molecular groups are given in the two appendixes. We show that the bond polarizability derivative model can quantitatively describe many aspects of the intensities observed in the SFG-VS spectrum of the vapour/neat liquid interfaces in different polarizations. Using the polarization analysis in SFG-VS, polarization selection rules or guidelines are developed for assignment of the SFG-VS spectrum. Using the selection rules, SFG-VS spectra of vapour/diol, and vapour/n-normal alcohol (n similar to 1-8) interfaces are assigned, and some of the ambiguity and confusion, as well as their implications in previous IR and Raman assignment, are duly discussed. The ability to assign a SFG-VS spectrum using the polarization selection rules makes SFG-VS not only an effective and useful vibrational spectroscopy technique for interface studies, but also a complementary vibrational spectroscopy method in general condensed phase studies. These developments will put quantitative orientational and spectral analysis in SFG-VS on a more solid foundation. The formulations, concepts and issues discussed in this review are expected to find broad applications for investigations on molecular interfaces in the future.
关键词[WOS]: AIR-WATER-INTERFACE ;  RAMAN TRACE SCATTERING ;  OPTICAL 2ND-HARMONIC GENERATION ;  LANGMUIR-BLODGETT MULTILAYERS ;  H STRETCHING VIBRATIONS ;  LIQUID-VAPOR INTERFACE ;  HARMONIC FORCE-FIELD ;  NORMAL-ALKYL CHAINS ;  MOLECULAR-ORIENTATION ;  INTENSITY PARAMETERS
语种: 英语
WOS记录号: WOS:000233115200001
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/139862
Appears in Collections:中国科学院大连化学物理研究所_期刊论文

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作者单位: 1.Chinese Acad Sci, Inst Chem, State Key Lab Mol React Dynam, Beijing 100080, Peoples R China

Recommended Citation:
Wang, HF,Gan, W,Lu, R,et al. Quantitative spectral and orientational analysis in surface sum frequency generation vibrational spectroscopy (SFG-VS)[J]. INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY,2005,24(2):191-256.
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