氮杂萘的激发态动力学揭示了合理设计光活性分子的机会。

IF 5.9 2区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Malcolm Garrow, Lauren Bertram, Abi Winter, Andrew W Prentice, Stuart W Crane, Paul D Lane, Stuart J Greaves, Martin J Paterson, Adam Kirrander, Dave Townsend
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引用次数: 0

摘要

各种光活性分子含有建立在杂环-芳杂环上的基序,尽管对这些系统中的激发态光物理和光化学的详细理解尚未充分发展。为了解决这一问题,利用超快瞬态吸收光谱研究了在己烷溶剂化下氮杂萘的非绝热动力学。具体来说,我们研究了喹啉、异喹啉、喹唑啉、喹诺啉、1,6-萘啶和1,8-萘啶,提供了双环芳烃结构中氮杂原子中心相对位置的系统变化。我们的结果表明激发态寿命,系统间交叉和分子系列内部转换的倾向有相当大的差异。整体的行为模式可以用势能势垒和自旋轨道耦合效应来解释,正如在SCS-ADC(2)理论水平上进行的大量量子化学计算所证明的那样。事实上,量子化学计算可以在六种分子的组成上表现出微妙的变化,从而与实验数据实现如此详细和微妙的一致,这为当前最先进的技术提供了一个很好的例子,并预示着未来合理设计光活性分子的机会。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Excited state dynamics of azanaphthalenes reveal opportunities for the rational design of photoactive molecules.

Various photoactive molecules contain motifs built on aza-aromatic heterocycles, although a detailed understanding of the excited state photophysics and photochemistry in such systems is not fully developed. To help address this issue, the non-adiabatic dynamics operating in azanaphthalenes under hexane solvation was studied following 267 nm excitation using ultrafast transient absorption spectroscopy. Specifically, the species quinoline, isoquinoline, quinazoline, quinoxaline, 1,6-naphthyridine, and 1,8-naphthyridine were investigated, providing a systematic variation in the relative positioning of nitrogen heteroatom centres within a bicyclic aromatic structure. Our results indicate considerable differences in excited state lifetimes, and in the propensity for intersystem crossing vs internal conversion across the molecular series. The overall pattern of behaviour can be explained in terms of potential energy barriers and spin-orbit coupling effects, as demonstrated by extensive quantum chemistry calculations undertaken at the SCS-ADC(2) level of theory. The fact that quantum chemistry calculations can achieve such detailed and nuanced agreement with experimental data across a full set of six molecules exhibiting subtle variations in their composition provides an excellent example of the current state-of-the-art and is indicative of future opportunities for rational design of photoactive molecules.

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来源期刊
Communications Chemistry
Communications Chemistry Chemistry-General Chemistry
CiteScore
7.70
自引率
1.70%
发文量
146
审稿时长
13 weeks
期刊介绍: Communications Chemistry is an open access journal from Nature Research publishing high-quality research, reviews and commentary in all areas of the chemical sciences. Research papers published by the journal represent significant advances bringing new chemical insight to a specialized area of research. We also aim to provide a community forum for issues of importance to all chemists, regardless of sub-discipline.
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