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Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution
Zhang, WK; Zheng, DS; Xu, YY; Bian, HT; Guo, Y; Wang, HF
刊名JOURNAL OF CHEMICAL PHYSICS
2005-12-08
DOI10.1063/1.2136875
123期:22
收录类别SCI
文章类型Review
WOS标题词Science & Technology ; Physical Sciences
类目[WOS]Physics, Atomic, Molecular & Chemical
研究领域[WOS]Physics
关键词[WOS]SUM-FREQUENCY GENERATION ; NONLINEAR-OPTICAL RESPONSE ; SURFACE-ADSORPTION LAYERS ; 2ND HARMONIC-GENERATION ; AIR-WATER-INTERFACE ; X-RAY REFLECTIVITY ; VAPOR INTERFACE ; VIBRATIONAL SPECTROSCOPY ; MOLECULAR-ORIENTATION ; MULTIPOLAR CONTRIBUTIONS
英文摘要It has been generally accepted that there are significant quadrupolar and bulk contributions to the second-harmonic generation (SHG) reflected from the neat air/water interface, as well as common liquid interfaces. Because there has been no general methodology to determine the quadrupolar and bulk contributions to the SHG signal from a liquid interface, this conclusion was reached based on the following two experimental phenomena: the breaking of the macroscopic Kleinman symmetry and the significant temperature dependence of the SHG signal from the neat air/water interface. However, because the sum frequency generation vibrational spectroscopy (SFG-VS) measurement of the neat air/water interface observed no apparent temperature dependence, the temperature dependence in the SHG measurement has been reexamined and proven to be an experimental artifact. Here we present a complete microscopic analysis of the susceptibility tensors of the air/water interface, and show that dipolar contribution alone can be used to address the issue of the breaking of the macroscopic Kleinman symmetry at the neat air/water interface. Using this analysis, the orientation of the water molecules at the interface can be obtained, and it is consistent with the measurement from SFG-VS. Therefore, the key rationales to conclude significantly quadrupolar and bulk contributions to the SHG signal of the neat air/water interface can no longer be considered as valid as before. This new understanding of the air/water interface can shed light on our understanding of the nonlinear optical responses from other molecular interfaces as well. (c) 2005 American Institute of Physics.
语种英语
WOS记录号WOS:000234120800044
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被引频次:40[WOS]   [WOS记录]     [WOS相关记录]
文献类型期刊论文
条目标识符http://cas-ir.dicp.ac.cn/handle/321008/139698
专题中国科学院大连化学物理研究所
作者单位Chinese Acad Sci, Inst Chem, State Key Lab Mol React Dynam, Beijing 100080, Peoples R China
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Zhang, WK,Zheng, DS,Xu, YY,et al. Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution[J]. JOURNAL OF CHEMICAL PHYSICS,2005,123(22).
APA Zhang, WK,Zheng, DS,Xu, YY,Bian, HT,Guo, Y,&Wang, HF.(2005).Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution.JOURNAL OF CHEMICAL PHYSICS,123(22).
MLA Zhang, WK,et al."Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution".JOURNAL OF CHEMICAL PHYSICS 123.22(2005).
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