Ultrafast motion in a third generation photomolecular motor.
Ultrafast motion in a third generation photomolecular motor.
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DOI：
10.1038/s41467-023-36777-6
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发表时间：
2023-03-06
影响因子：
16.6
通讯作者：
Meech, Stephen R.
中科院分区：
文献类型：
--
作者：
Roy, Palas;Browne, Wesley R.;Feringa, Ben L.;Meech, Stephen R.
在纳米尺度上控制分子翻译是合成分子机器发展的一个关键目标。最近开发的第三代光化学驱动分子马达（3GMs），由能够单向协作旋转的过度拥挤的烯烃对组成，提供了将光能转化为平动运动的可能性。3gm的进一步发展需要详细了解其激发态动力学。在这里，我们使用时间分辨吸收和发射来跟踪3GM中的种群和相干动力学。飞秒激发拉曼揭示了激发态从Franck-Condon亮态到弱发射暗态到亚稳态产物的实时结构动力学，为反应坐标提供了新的见解。溶剂极性改变了光转换效率，表明暗态下的电荷转移特性。增强的量子产率与抑制激发态的低频扑动有关。这种详细的表征促进了3gm的发展，表明利用介质和取代基效应来调节电机效率。在纳米尺度上控制分子运动对纳米机械的设计具有重要意义。在这里，作者使用超快振动和电子能谱来表征设计用于支持平移运动的光驱动分子马达的运动机制。
Controlling molecular translation at the nanoscale is a key objective for development of synthetic molecular machines. Recently developed third generation photochemically driven molecular motors (3GMs), comprising pairs of overcrowded alkenes capable of cooperative unidirectional rotation offer the possibility of converting light energy into translational motion. Further development of 3GMs demands detailed understanding of their excited state dynamics. Here we use time-resolved absorption and emission to track population and coherence dynamics in a 3GM. Femtosecond stimulated Raman reveals real-time structural dynamics as the excited state evolves from a Franck-Condon bright-state through weakly-emissive dark-state to the metastable product, yielding new insight into the reaction coordinate. Solvent polarity modifies the photoconversion efficiency suggesting charge transfer character in the dark-state. The enhanced quantum yield correlates with suppression of a low-frequency flapping motion in the excited state. This detailed characterization facilitates development of 3GMs, suggesting exploitation of medium and substituent effects to modulate motor efficiency. Controlling molecular motion at nanoscale is important for the design of nanomachines. Here the authors use ultrafast vibrational and electronic spectroscopy to characterize the mechanism of motion of a light driven molecular motor designed to support translational movement.
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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
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：
2.9
作者：
Lee, Gyeongjin;Kim, Junwoo;Joo, Taiha
通讯作者：
Joo, Taiha
影响因子：
15
作者：
Liu, Fengyi;Morokuma, Keiji
通讯作者：
Morokuma, Keiji
影响因子：
2.9
作者：
Amirjalayer, Saeed;Cnossen, Arjen;Browne, Wesley R.;Feringa, Ben L.;Buma, Wybren J.;Woutersen, Sander
通讯作者：
Woutersen, Sander