穆勒矩阵偏振法揭示了溶液中金属螯合物的热性

IF 4.3 2区 化学 Q1 SPECTROSCOPY
Daniel Vala , Jiří Zdráhala , Jana Hudecová , Hana Šestáková , Jaroslav Šebestík , David Kopečný , Josef Kapitán , Petr Bouř , Kamil Postava
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引用次数: 0

摘要

分子热学性质的正确表征对有机化学和药物开发至关重要。然而,狭窄的光谱范围和专用设备的必要性往往限制了传统的方法,如光学旋转色散和电子圆二色性。在这里,我们介绍穆勒矩阵偏振法(MMP)作为一个更通用的工具,用于色光分析,能够同时捕获圆二色性和旋光色散光谱跨越紫外至近红外波长在一个单一的测量。我们将MMP应用于Al, Mn和Co的手性金属配合物,这些配合物通常用作不对称合成的催化剂。使用稳健的实验方法,MMP区分了对映体形式,并通过利用圆二色性和光旋色散之间的固有关系提供了可靠的色散信息。我们在密度泛函理论模拟的基础上解释了我们的发现,将它们与传统的电子圆二色性和吸收光谱进行了比较,并进行了Kramers-Kronig分析。例如,热风MMP和ab-initio的结合方法揭示了中性钴金属配合物的精细近红外热风光谱。虽然MMP更常用于固态,但开发的实验协议显着扩展了其解决方案的能力。它允许在不需要对映体的情况下进行测量,并为分子手性提供了新的见解,具有跨传统和跨学科科学和工业分支的潜在应用。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Mueller matrix polarimetry reveals chiroptical properties of metal chelates in solutions

Mueller matrix polarimetry reveals chiroptical properties of metal chelates in solutions
Proper characterization of molecular chiroptical properties is vital for organic chemistry and drug development. Nonetheless, narrow spectral ranges and the necessity for specialized equipment often limit traditional methods such as optical rotatory dispersion and electronic circular dichroism. Here, we introduce Mueller matrix polarimetry (MMP) as a more versatile tool for chiroptical analysis, capable of simultaneously capturing circular dichroism and optical rotatory dispersion spectra across ultraviolet to near-infrared wavelengths in a single measurement. We applied MMP to chiral metal complexes of Al, Mn, and Co, commonly used as catalysts in asymmetric syntheses. Using a robust experimental methodology, MMP distinguished enantiomeric forms and provided reliable chiroptical information by leveraging the inherent relationship between circular dichroism and optical rotatory dispersion. We interpreted our findings on the basis of density functional theory simulations, compared them to traditional electronic circular dichroism and absorption spectroscopies, and performed the Kramers-Kronig analysis. The combined approach of chiroptical MMP and ab-initio, for example, reveals delicate near-infrared chiroptical spectra of a neutral cobalt metal complex. Although MMP is more commonly used for solid state, the developed experimental protocol significantly expands its capabilities to solutions. It allows measurements without the need for both enantiomers and offers new insights into molecular chirality with potential applications across traditional and interdisciplinary branches of science and industry.
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来源期刊
CiteScore
8.40
自引率
11.40%
发文量
1364
审稿时长
40 days
期刊介绍: Spectrochimica Acta, Part A: Molecular and Biomolecular Spectroscopy (SAA) is an interdisciplinary journal which spans from basic to applied aspects of optical spectroscopy in chemistry, medicine, biology, and materials science. The journal publishes original scientific papers that feature high-quality spectroscopic data and analysis. From the broad range of optical spectroscopies, the emphasis is on electronic, vibrational or rotational spectra of molecules, rather than on spectroscopy based on magnetic moments. Criteria for publication in SAA are novelty, uniqueness, and outstanding quality. Routine applications of spectroscopic techniques and computational methods are not appropriate. Topics of particular interest of Spectrochimica Acta Part A include, but are not limited to: Spectroscopy and dynamics of bioanalytical, biomedical, environmental, and atmospheric sciences, Novel experimental techniques or instrumentation for molecular spectroscopy, Novel theoretical and computational methods, Novel applications in photochemistry and photobiology, Novel interpretational approaches as well as advances in data analysis based on electronic or vibrational spectroscopy.
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