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Spectral Tuning and Photoisomerization Efficiency in Push–Pull Azobenzenes: Designing Principles
The Journal of Physical Chemistry A ( IF 2.9 ) Pub Date : 2020-11-10 , DOI: 10.1021/acs.jpca.0c08672 Flavia Aleotti 1 , Artur Nenov 1 , Luca Salvigni 1 , Matteo Bonfanti 1 , Mohsen M. El-Tahawy 1, 2 , Andrea Giunchi 1 , Marziogiuseppe Gentile 3 , Claudia Spallacci 1 , Alessia Ventimiglia 1 , Giuseppe Cirillo 1 , Lorenzo Montali 1 , Stefano Scurti 1 , Marco Garavelli 1 , Irene Conti 1
The Journal of Physical Chemistry A ( IF 2.9 ) Pub Date : 2020-11-10 , DOI: 10.1021/acs.jpca.0c08672 Flavia Aleotti 1 , Artur Nenov 1 , Luca Salvigni 1 , Matteo Bonfanti 1 , Mohsen M. El-Tahawy 1, 2 , Andrea Giunchi 1 , Marziogiuseppe Gentile 3 , Claudia Spallacci 1 , Alessia Ventimiglia 1 , Giuseppe Cirillo 1 , Lorenzo Montali 1 , Stefano Scurti 1 , Marco Garavelli 1 , Irene Conti 1
Affiliation
This work demonstrates how push–pull substitution can induce spectral tuning toward the visible range and improve the photoisomerization efficiency of azobenzene-based photoswitches, making them good candidates for technological and biological applications. The red-shifted bright ππ* state (S2) behaves like the lower and more productive dark nπ* (S1) state because less potential energy along the planar bending mode is available to reach higher energy unproductive nπ*/S0 crossing regions, which are responsible for the lower quantum yield of the parent compound. The stabilization of the bright ππ* state and the consequent increase in isomerization efficiency may be regulated via the strength of push–pull substituents. Finally, the torsional mechanism is recognized here as the unique productive route because structures with bending values attributable to the inversion mechanism were never detected, out of the 280 ππ* time-dependent density functional theory (RASPT2-validated) dynamics simulations.
中文翻译:
推挽式偶氮苯的光谱调谐和光异构化效率:设计原理
这项工作演示如何推-拉替代可诱导朝可见光谱范围内调整和完善基于偶氮苯的光电继电器的光致异构化效率,使他们的技术和生物应用的良好候选者。红移的亮ππ*状态(S 2)的行为类似于较低且生产率更高的暗nπ*(S 1)状态,因为沿平面弯曲模式的势能较小,可以达到较高的能量非生产率nπ* / S 0穿越区域,这是母体化合物较低的量子产率的原因。亮ππ*状态的稳定化和随之而来的异构化效率的提高可通过实力推-拉取代。最后,在280ππ*时变密度泛函理论(经过RASPT2验证)的动力学模拟中,扭转机制在这里被认为是唯一的生产路线,因为从未发现具有归因于扭转机制的弯曲值的结构。
更新日期:2020-11-19
中文翻译:
推挽式偶氮苯的光谱调谐和光异构化效率:设计原理
这项工作演示如何推-拉替代可诱导朝可见光谱范围内调整和完善基于偶氮苯的光电继电器的光致异构化效率,使他们的技术和生物应用的良好候选者。红移的亮ππ*状态(S 2)的行为类似于较低且生产率更高的暗nπ*(S 1)状态,因为沿平面弯曲模式的势能较小,可以达到较高的能量非生产率nπ* / S 0穿越区域,这是母体化合物较低的量子产率的原因。亮ππ*状态的稳定化和随之而来的异构化效率的提高可通过实力推-拉取代。最后,在280ππ*时变密度泛函理论(经过RASPT2验证)的动力学模拟中,扭转机制在这里被认为是唯一的生产路线,因为从未发现具有归因于扭转机制的弯曲值的结构。