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| A Simplified Method of Microscopic Polarizability Tensor Differential of Hyper-Raman Spectroscopy Based on Experimental Correction Bond Additivity Model-C2v Symmetry |
| WANG Yuan1, ZHANG Zhen2*, GUO Yuan2, 3 |
1. Institute of Technology, University of Sanya, Sanya 572022, China
2. Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences, Beijing 100010, China
3. School of Chemical Sciences, University of Chinese Academy of Sciences, Beijing 100049, China |
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Abstract Coherent Anti-Stokes Raman Spectroscopy (CARS) and Coherent Anti-Stokes Hyper-Raman Spectroscopy (CAHRS), as the high-order nonlinear spectroscopy techniques, have been used in many research studies fields such as dynamic process, gene expression spectrum screening, and high-resolution spectroscopy. However, it is difficult to make a quantitative analysis of the spectral signals that involved many high-order micro-polarizability tensors. It has reported that the CARS and CAHRS microscopic hyperpolarizability tensor elements can be decomposed into the product of the differentiation of Raman microscopic polarizability tensor α′i′j′ and Hyper-Raman microscopic polarizability tensor β′i′j′k′ which simplifies the difficulty of quantitative analysis of higher-order spectra to the analysis of lower-order spectra. In this paper, we use the bond additivity model (BAM) combined with the experimental correction to address the C2v symmetry molecular and present the simplified scheme for differentiation of Hyper-Raman microscopic polarizability tensor elements β′i′j′k′. The differentiation of Hyper-Raman microscopic polarizability tensor elements β′i′j′k′ of the C2v molecular group is obtained and the expressions of β′i′j′k′ for symmetric and antisymmetric vibrations of the C2v molecular group also are deduced. According to the experimental measurement of the Hyper-Raman spectral intensity ratio of different polarization combinations of the ρHR-SS and ρHR-AS, along with HV polarization combinations of the corresponding vibration modes, the ratio between β′i′j′k′ of C2v molecular group modified by Hyper-Raman experiment is obtained. Finally, substituting the experimentally corrected differentiation of Raman microscopic polarizability tensor elements α′i′j′ in the literature into the ratio above can obtain the proportional relationship between CARS the microscopic polarizability tensor elements and CAHRS of the C2v molecular group. This method can provide the basis for the quantitative analysis of high-order nonlinear spectral.
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Received: 2020-12-24
Accepted: 2021-03-19
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Corresponding Authors:
ZHANG Zhen
E-mail: zhangz@iccas.ac.cn
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| [1] |
WANG Yuan1, ZHANG Zhen2*, GUO Yuan2, 3. A Simplified Method of Microscopic Hyperpolarizability of Coherent Anti-Stokes Raman Spectroscopy and Coherent Anti-Stokes Hyper-Raman Spectroscopy-C3v Symmetry[J]. SPECTROSCOPY AND SPECTRAL ANALYSIS, 2020, 40(05): 1382-1387. |
| [2] |
WANG Yuan1, ZHANG Zhen2*, GUO Yuan2, 3. A Simplified Method of Microscopic Hyperpolarizability of Coherent Anti-Stokes Raman Spectroscopy and Coherent Anti-Stokes Hyper-Raman Spectroscopy-C∞v Symmetry[J]. SPECTROSCOPY AND SPECTRAL ANALYSIS, 2019, 39(02): 465-470. |
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