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弱束缚络合物中手性分子的微波三波混频光谱学

Microwave Three-Wave Mixing Spectroscopy of Chiral Molecules in Weakly Bound Complexes.

作者信息

Sun Wenhao, Schnell Melanie

机构信息

Deutsches Elektronen-Synchrotron DESY, Notkestr. 85, 22607 Hamburg, Germany.

Institute of Physical Chemistry, Christian-Albrechts-Universität zu Kiel, Max-Eyth-Strasse 1, 24118 Kiel, Germany.

出版信息

J Phys Chem Lett. 2023 Aug 24;14(33):7389-7394. doi: 10.1021/acs.jpclett.3c01900. Epub 2023 Aug 11.

DOI:10.1021/acs.jpclett.3c01900
PMID:37566689
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC10461301/
Abstract

Since the first experimental implementation in 2013, microwave three-wave mixing has emerged as a robust spectroscopic approach for analyzing and controlling chiral molecules in the gas phase. This resonant, coherent, and nonlinear technique is based on the three-dimensional light-matter interaction in the electric dipole approximation, allowing for isomer- and conformer-selective chiral analysis with high resolution. Here we demonstrate the utility of microwave three-wave mixing for analyzing a molecular complex, limonene-HO, which serves as a compelling example of addressing its potential to improve the chiral sensitivity for only weakly polar chiral molecules. The use of molecular complexes can also extend the applicability of microwave three-wave mixing to chiral systems that are not in the point group.

摘要

自2013年首次实验实现以来,微波三波混频已成为一种用于分析和控制气相手性分子的强大光谱方法。这种共振、相干和非线性技术基于电偶极近似下的三维光与物质相互作用,能够实现高分辨率的异构体和构象体选择性手性分析。在此,我们展示了微波三波混频在分析分子复合物柠檬烯-HO中的应用,该复合物是提高仅弱极性手性分子手性灵敏度潜力的一个有说服力的例子。分子复合物的使用还可以将微波三波混频的适用性扩展到不属于 点群的手性系统。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/c282bcf6e4ce/jz3c01900_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/dc8bc562bc33/jz3c01900_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/457f9bf23594/jz3c01900_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/6f57c7db36cd/jz3c01900_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/d516f5d4dff8/jz3c01900_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/c282bcf6e4ce/jz3c01900_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/dc8bc562bc33/jz3c01900_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/457f9bf23594/jz3c01900_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/6f57c7db36cd/jz3c01900_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/d516f5d4dff8/jz3c01900_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/60cc/10461301/c282bcf6e4ce/jz3c01900_0005.jpg

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本文引用的文献

1
Chiral Control of Gas-Phase Molecules using Microwave Pulses.使用微波脉冲对气相分子进行手性控制。
Angew Chem Int Ed Engl. 2023 Jul 3;62(27):e202219045. doi: 10.1002/anie.202219045. Epub 2023 Apr 27.
2
Accuracy of quantum chemistry structures of chiral tag complexes and the assignment of absolute configuration.手性标签配合物量子化学结构的准确性及绝对构型的指定
Phys Chem Chem Phys. 2022 Nov 23;24(45):27705-27721. doi: 10.1039/d2cp04060c.
3
Quantitative Study of Enantiomer-Specific State Transfer.对映体特异性态转移的定量研究。
Phys Rev Lett. 2022 Apr 29;128(17):173001. doi: 10.1103/PhysRevLett.128.173001.
4
New Insights into Secondary Organic Aerosol Formation: Water Binding to Limonene.二次有机气溶胶形成的新见解:水与柠檬烯的结合
J Phys Chem Lett. 2021 Jan 28;12(3):1081-1086. doi: 10.1021/acs.jpclett.0c03574. Epub 2021 Jan 20.
5
Rapid quantification of isomeric and dehalogenated impurities in pharmaceutical raw materials using MRR spectroscopy.采用分子旋转共振光谱法快速定量药物原料中的同分异构体和脱卤杂质。
J Pharm Biomed Anal. 2020 Sep 10;189:113474. doi: 10.1016/j.jpba.2020.113474. Epub 2020 Jul 17.
6
Water Docking Bias in [4]Helicene.[4]螺旋烯中的水对接偏差
Angew Chem Int Ed Engl. 2019 Aug 12;58(33):11257-11261. doi: 10.1002/anie.201902889. Epub 2019 Jul 4.
7
Influence of spatial degeneracy on rotational spectroscopy: Three-wave mixing and enantiomeric state separation of chiral molecules.空间简并对旋转光谱的影响:手性分子的三波混频和对映异构体态分离。
J Chem Phys. 2018 Sep 7;149(9):094201. doi: 10.1063/1.5045052.
8
State-Specific Enrichment of Chiral Conformers with Microwave Spectroscopy.利用微波光谱对特定状态下的手性构象体进行富集
J Phys Chem Lett. 2018 Aug 16;9(16):4539-4543. doi: 10.1021/acs.jpclett.8b01815. Epub 2018 Jul 31.
9
Chiral pharmaceuticals: A review on their environmental occurrence and fate processes.手性药物:环境赋存及归趋过程研究综述。
Water Res. 2017 Nov 1;124:527-542. doi: 10.1016/j.watres.2017.08.003. Epub 2017 Aug 5.
10
Coherent Enantiomer-Selective Population Enrichment Using Tailored Microwave Fields.利用定制微波场实现相干对映体选择性布居数富集。
Angew Chem Int Ed Engl. 2017 Oct 2;56(41):12512-12517. doi: 10.1002/anie.201704901. Epub 2017 Aug 2.