腙衍生物分子开关的光致异构化机理研究。

IF 4.3 3区 化学 Q2 CHEMISTRY, MULTIDISCIPLINARY
ACS Omega Pub Date : 2025-04-23 eCollection Date: 2025-05-06 DOI:10.1021/acsomega.5c00820
Xiaojuan Pang, Kaiyue Zhao, Chenghao Yang, Quanjie Zhong, Ningbo Zhang, Chenwei Jiang
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引用次数: 0

摘要

提高量子产率是提高光驱动分子马达运行效率的重要特征。基于Cigan等人在CH3取代H (RSC Adv., 2015, 5,62449)方面的开创性工作,我们通过用两个氢原子取代单个氧原子,开发了一种基于腙的分子开关的结构修饰策略,从而显著提高了量子产率。在半经验OM2/MRCI水平上,利用Tully表面跳变方法系统地研究了腙衍生物分子开关的光致异构化机理。结果表明,该分子旋转电机E-to-Z光异构的计算量子产率约为(55±3)%(原(Pang, x.j .;赵、K.-Y;他,H.-Y。;张,不可开交。江,C.-W。isatin n2 -二苯腙分子开关的光诱导异构化机理。《物理学》。原子学报,2024,73(17).),激发态的平均寿命为122fs。此外,我们计算了随时间变化的荧光发射光谱,观察到波长红移伴随着荧光发射猝灭,与原始的isatin - n2 - diphenylhydra腙光谱相比,显示出蓝移。此外,我们提出这种分子开关可能没有“暗态”。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Study on the Photoinduced Isomerization Mechanism of Hydrazone Derivatives Molecular Switch.

Study on the Photoinduced Isomerization Mechanism of Hydrazone Derivatives Molecular Switch.

Study on the Photoinduced Isomerization Mechanism of Hydrazone Derivatives Molecular Switch.

Study on the Photoinduced Isomerization Mechanism of Hydrazone Derivatives Molecular Switch.

Improving quantum yield is an important characteristic for enhancing the operational efficiency of light-driven molecular motors. Building upon Cigan et al.'s pioneering work on CH3 substitution for H (RSC Adv., 2015, 5, 62449), we have developed a structural modification strategy for hydrazone-based molecular switches through the replacement of a single oxygen atom with two hydrogen atoms, resulting in a remarkable enhancement of the quantum yield. We systematically investigate the photoinduced isomerization mechanism of the hydrazone derivatives molecular switch using the Tully's surface hopping method on the semiempirical OM2/MRCI level. The results show that the calculated quantum yield for the E-to-Z photoisomerization of this molecular rotary motor is approximately (55 ± 3)% (16.01% for original (Pang, X.-J.; Zhao, K.-Y.; He, H.-Y.; Zhang, N.-B.; Jiang, C.-W. Photoinduced isomerization mechanism of isatin N2-diphenylhydrazones molecular switch. Acta Phys. Sin. 2024, 73 (17).) with an average lifetime of the excited state of 122 fs. Additionally, we calculate the time-dependent fluorescence emission spectra and observe a redshift in wavelength accompanied by fluorescence emission quenching, which shows a blue shift compared to the original isatin N2-diphenylhydrazone spectrum. Furthermore, we propose that this molecular switch may not have a "dark state".

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来源期刊
ACS Omega
ACS Omega Chemical Engineering-General Chemical Engineering
CiteScore
6.60
自引率
4.90%
发文量
3945
审稿时长
2.4 months
期刊介绍: ACS Omega is an open-access global publication for scientific articles that describe new findings in chemistry and interfacing areas of science, without any perceived evaluation of immediate impact.
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