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NEXMD Modeling of Photoisomerization Dynamics of 4-Styrylquinoline
The Journal of Physical Chemistry A ( IF 2.9 ) Pub Date : 2018-11-02 00:00:00 , DOI: 10.1021/acs.jpca.8b09103 Andrew E. Sifain 1, 2 , Brendan J. Gifford 2 , David W. Gao 2, 3 , Levi Lystrom 2, 4 , Tammie R. Nelson 2 , Sergei Tretiak 2, 5
The Journal of Physical Chemistry A ( IF 2.9 ) Pub Date : 2018-11-02 00:00:00 , DOI: 10.1021/acs.jpca.8b09103 Andrew E. Sifain 1, 2 , Brendan J. Gifford 2 , David W. Gao 2, 3 , Levi Lystrom 2, 4 , Tammie R. Nelson 2 , Sergei Tretiak 2, 5
Affiliation
Isomerization of molecular systems is ubiquitous in chemistry and biology, and is also important for many applications. Atomistic simulations can help determine the tunable parameters influencing this process. In this paper, we use the Nonadiabatic EXcited state Molecular Dynamics (NEXMD) software to study the photoisomerization of a representative molecule, 4-styrylquinoline (SQ). trans-SQ transforms into dihydrobenzophenanthridine (DHBP) upon irradiation with laser light, with the cis conformer acting as an intermediate. We study how varying three different external stimuli (i.e., apolar versus polar solvent, low versus high photoexcitation energy, and vacuum versus a constant temperature thermostat) affects the trans-to-cis photoisomerization of SQ. Our results show that polarization effects due to implicit solvation and the thermostat play a crucial role in the isomerization process, whereas photoexcitation energy plays a lesser role on the outcome and efficiency. We also show that NEXMD captures the correct energy profile between the ground and first singlet excited state, showing that there are two distinct reaction pathways to the final stable product that vary by the number of photons absorbed, in agreement with experiment. Ultimately, NEXMD proves to be an effective tool for investigating excited state single molecule dynamics subject to various environments and initial conditions.
中文翻译:
NEXMD建模的4-苯乙烯基喹啉的光致异构动力学
分子系统的异构化在化学和生物学中无处不在,并且对于许多应用也很重要。原子模拟可以帮助确定影响此过程的可调参数。在本文中,我们使用非绝热激发态分子动力学(NEXMD)软件来研究代表性分子4-苯乙烯基喹啉(SQ)的光异构化。反式-SQ在激光照射下转变为二氢苯并菲(DHBP),顺式构象体充当中间体。我们研究如何变化的三种不同的外部刺激(即,非极性与极性溶剂,低与高光激发能量,相对于真空的恒温恒温器)会影响反式-到-顺SQ的光异构化。我们的结果表明,由于隐性溶剂化和恒温器引起的极化效应在异构化过程中起关键作用,而光激发能对结果和效率的作用较小。我们还表明,NEXMD捕获了基态和第一个单重态激发态之间的正确能量分布,表明与最终实验结果一致,有两种截然不同的反应途径随吸收的光子数量的不同而变化。最终,证明NEXMD是研究受各种环境和初始条件影响的激发态单分子动力学的有效工具。
更新日期:2018-11-02
中文翻译:
NEXMD建模的4-苯乙烯基喹啉的光致异构动力学
分子系统的异构化在化学和生物学中无处不在,并且对于许多应用也很重要。原子模拟可以帮助确定影响此过程的可调参数。在本文中,我们使用非绝热激发态分子动力学(NEXMD)软件来研究代表性分子4-苯乙烯基喹啉(SQ)的光异构化。反式-SQ在激光照射下转变为二氢苯并菲(DHBP),顺式构象体充当中间体。我们研究如何变化的三种不同的外部刺激(即,非极性与极性溶剂,低与高光激发能量,相对于真空的恒温恒温器)会影响反式-到-顺SQ的光异构化。我们的结果表明,由于隐性溶剂化和恒温器引起的极化效应在异构化过程中起关键作用,而光激发能对结果和效率的作用较小。我们还表明,NEXMD捕获了基态和第一个单重态激发态之间的正确能量分布,表明与最终实验结果一致,有两种截然不同的反应途径随吸收的光子数量的不同而变化。最终,证明NEXMD是研究受各种环境和初始条件影响的激发态单分子动力学的有效工具。