Reconsideration of second-harmonic generation from isotropic liquid interface: Broken Kleinman symmetry of neat air/water interface from dipolar contribution

doi:10.1063/1.2136875

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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
卷号	123 期号:22
ISSN号	0021-9606
DOI	10.1063/1.2136875
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
出版者	AMER INST PHYSICS
WOS记录号	WOS:000234120800044
内容类型	期刊论文
源URL	[http://ir.iccas.ac.cn/handle/121111/56405]
专题	中国科学院化学研究所
通讯作者	Wang, HF
作者单位	Chinese Acad Sci, Inst Chem, State Key Lab Mol React Dynam, Beijing 100080, Peoples R China
推荐引用方式 GB/T 7714	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).