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

	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
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.
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
收录类别	SCI
语种	英语
WOS记录号	WOS:000234120800044
公开日期	2015-11-10
内容类型	期刊论文
源URL	[http://159.226.238.44/handle/321008/139698]
专题	大连化学物理研究所_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
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).