Control of Photoconversion Yield in Unidirectional Photomolecular Motors by Push-Pull Substituents.
Control of Photoconversion Yield in Unidirectional Photomolecular Motors by Push-Pull Substituents.
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DOI：
10.1021/jacs.3c06070
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发表时间：
2023-09-13
影响因子：
15
通讯作者：
Meech, Stephen R.
中科院分区：
文献类型：
--
作者：
Roy, Palas;Sardjan, Andy S.;Danowski, Wojciech;Browne, Wesley R.;Feringa, Ben L.;Meech, Stephen R.
基于过度拥挤的烯烃基序的分子马达通过激发态异构化反应将光能转化为单向机械运动。实现对这些分子马达转换效率的实验控制是一个重要目标。在这里，我们将新型“推拉”过度拥挤烯烃发动机的合成与稳态和超快时间分辨电子光谱的光物理表征结合起来。我们表明，激发态电荷转移特性的调节对光异构化产率具有显着影响，在非极性溶剂中将其增强至接近统一，而在极性溶剂中则很大程度上抑制它。这种行为是通过参考溶剂和取代基相关的势能表面及其对基态圆锥相交的影响来解释的。这些观察结果为精细控制电机效率提供了新途径，并为光驱动分子电机的合成和开发引入了额外的自由度。
Molecular motors based on the overcrowded alkene motif convert light energy into unidirectional mechanical motion through an excited state isomerization reaction. The realization of experimental control over conversion efficiency in these molecular motors is an important goal. Here, we combine the synthesis of a novel “push–pull” overcrowded alkene motor with photophysical characterization by steady state and ultrafast time-resolved electronic spectroscopy. We show that tuning of the charge transfer character in the excited state has a dramatic effect on the photoisomerization yield, enhancing it to near unity in nonpolar solvents while largely suppressing it in polar solvents. This behavior is explained through reference to solvent- and substituent-dependent potential energy surfaces and their effect on conical intersections to the ground state. These observations offer new routes to the fine control of motor efficiency and introduce additional degrees of freedom in the synthesis and exploitation of light-driven molecular motors.
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DOI：
10.1021/acs.jpclett.5b02575
发表时间：
2016-01-07
期刊：
The journal of physical chemistry letters
影响因子：
--
作者：
Nikiforov A;Gamez JA;Thiel W;Filatov M
通讯作者：
Filatov M
影响因子：
15
作者：
Kistemaker JCM;Štacko P;Roke D;Wolters AT;Heideman GH;Chang MC;van der Meulen P;Visser J;Otten E;Feringa BL
通讯作者：
Feringa BL
影响因子：
3.2
作者：
Pollard, Michael M.;Meetsma, Auke;Feringa, Ben L.
通讯作者：
Feringa, Ben L.
影响因子：
15
作者：
Liu, Fengyi;Morokuma, Keiji
通讯作者：
Morokuma, Keiji
影响因子：
4.4
作者：
Malhado, Joao Pedro;Hynes, James T.
通讯作者：
Hynes, James T.