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题名: Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution
作者: Zhang, WK;  Zheng, DS;  Xu, YY;  Bian, HT;  Guo, Y;  Wang, HF
刊名: JOURNAL OF CHEMICAL PHYSICS
发表日期: 2005-12-08
DOI: 10.1063/1.2136875
卷: 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
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.
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
语种: 英语
WOS记录号: WOS:000234120800044
Citation statistics: 
内容类型: 期刊论文
URI标识: http://cas-ir.dicp.ac.cn/handle/321008/139698
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:
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).
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