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Experimental Observables and Macroscopic Susceptibility/Microscopic Polarizability Tensors for Third and Fourth-Order Nonlinear Spectroscopy of Ordered Molecular System
Yuan Wang,Zhi-feng Cui*,Hong-fei Wang*
Author NameAffiliationE-mail
Yuan Wang Department of Physics, Anhui Normal University, Wuhu 241000, China  
Zhi-feng Cui* Department of Physics, Anhui Normal University, Wuhu 241000, China zfcui@mail.ahnu.edu.cn 
Hong-fei Wang* Department of Physics, Anhui Normal University, Wuhu 241000, China; State Key Laboratory of Molecular Reaction Dynamics, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100080, China hongfei@iccas.ac.cn 
Abstract:
There has been emerging needs for the quantitative polarization analysis for the Coherent Anti-stokes Raman Spectroscopy and Coherent Anti-stokes Hyper-raman Spectroscopy, as the experimental studies with coherent anti-stokes raman spectroscopy and coherent anti-stokes hyper-raman spectroscopy for the interface and membrane studies being growing. Recently we have demonstrated that orientational analysis of linear and nonlinear spectroscopy from the ordered molecular system, such as molecular interfaces and ˉlms, can be carried out with the formulation of the orientational function in simple functional forms. Applications of such formulation for the second order spectroscopy, namely, the Second Harmonic Generation and Sum Frequency Generation Vibrational Spectroscopy, have helped to understand spectral and orientational details of the molecular interfaces and ˉlms. In order to employ this formulation for the higher order coherent nonlinear spectroscopy, the detailed expressions of the experimental observables and the macroscopic sus- ceptibility/microscopic polarizability tensors for the third and fourth-order nonlinear spectroscopy for the interface or ˉlm is presented with the rotational symmetry. General expressions for the typical third and fourth order spectroscopy, such as the Third Harmonic Generation, the degenerated coherent anti-stokes raman spectroscopy, the Fourth Harmonic Generation and the degenerated coherent anti-stokes hyper-raman spectroscopy, are presented for their future applications. The advantages and limitations of the third and fourth order spectroscopic techniques are also discussed.
Key words:  Third and fourth-order nonlinear spectroscopy, Experimental observable, Macroscopic susceptibility/microscopic polarizability tensor, Ordered molecular system
FundProject:国家重点实验室
有序分子体系的三阶和四阶非线性光谱学的实验可观测量和宏观感应率及微观极化率张量元
汪源,崔执凤*,王鸿飞*
摘要:
对于线性和非线性光谱,有序的分子体系(如分子界面和分子膜)的取向分析可以通过对形式非常简单的广义取向泛函.对于二阶非线性光谱学,即光学二次谐波和和频振动光谱,这一简化描述对于理解分子界面和膜的光谱和取向的细节很有助益.为了将这一简化描述应用于更高阶的相干非线性光谱学,对于具有旋转对称性的界面或膜的三阶和四阶非线性光谱学的实验可观测量和宏观感应率及微观极化率张量元进行了计算并得到了具体表达式.这些通用的表达式将有助于典型的三、四阶非线性光谱学,即光学三次谐波、简并的相干反斯托克斯拉曼光谱、光学四次谐波和简并
关键词:  非线性光谱学,实验可观测量,宏观感应率和微观极化率张量,有序分子体系
DOI:10.1088/1674-0068/20/04/449-460
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