Perylene-derivative singlet exciton fission in water solution

IF 7.6 1区化学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Chemical Science Pub Date : 2024-10-04 DOI:10.1039/d4sc04732j

Chloe MAGNE, Simona Streckaitė, Roberto Boto, Eduardo Domínguez-Ojeda, Marina Gromova, Andrea Echeverri, Flavio Siro Brigiano, Minh-Huong Ha-Thi, Marius Franckevičius, Vidmantas Jašinskas, Annamaria Quaranta, Andrew A. Pascal, Matthieu Koepf, David Casanova, Thomas Pino, Bruno Robert, Julia Contreras-García, Daniel Finkelstein Shapiro, Vidmantas Gulbinas, Manuel J. Llansola-Portoles

{"title":"Perylene-derivative singlet exciton fission in water solution","authors":"Chloe MAGNE, Simona Streckaitė, Roberto Boto, Eduardo Domínguez-Ojeda, Marina Gromova, Andrea Echeverri, Flavio Siro Brigiano, Minh-Huong Ha-Thi, Marius Franckevičius, Vidmantas Jašinskas, Annamaria Quaranta, Andrew A. Pascal, Matthieu Koepf, David Casanova, Thomas Pino, Bruno Robert, Julia Contreras-García, Daniel Finkelstein Shapiro, Vidmantas Gulbinas, Manuel J. Llansola-Portoles","doi":"10.1039/d4sc04732j","DOIUrl":null,"url":null,"abstract":"We provide direct evidence of singlet fission occurring with water-soluble compounds. We show that perylene-3,4,9,10-tetracarboxylate forms dynamic dimers in aqueous solution, with lifetimes long enough to allow intermolecular processes such as singlet fission. As these are transient dimers rather than stable aggregates, they retain a significant degree of disorder. We performed a comprehensive analysis of such dynamic assemblies using time-resolved absorption and fluorescence spectroscopy, nuclear magnetic resonance spectroscopy, and theoretical modelling, allowing us to observe the characteristic signatures of singlet fission and develop a model to characterize the different species observed. Our findings reveal that structure fluctuations within perylene-3,4,9,10-tetracarboxylate associations are key in favoring either singlet fission or charge separation. The efficiency of triplet formation is higher than 100%, and the disordered system leads to triplets living in the nanosecond time range.","PeriodicalId":9909,"journal":{"name":"Chemical Science","volume":null,"pages":null},"PeriodicalIF":7.6000,"publicationDate":"2024-10-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Science","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1039/d4sc04732j","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}

引用次数: 0

Abstract

We provide direct evidence of singlet fission occurring with water-soluble compounds. We show that perylene-3,4,9,10-tetracarboxylate forms dynamic dimers in aqueous solution, with lifetimes long enough to allow intermolecular processes such as singlet fission. As these are transient dimers rather than stable aggregates, they retain a significant degree of disorder. We performed a comprehensive analysis of such dynamic assemblies using time-resolved absorption and fluorescence spectroscopy, nuclear magnetic resonance spectroscopy, and theoretical modelling, allowing us to observe the characteristic signatures of singlet fission and develop a model to characterize the different species observed. Our findings reveal that structure fluctuations within perylene-3,4,9,10-tetracarboxylate associations are key in favoring either singlet fission or charge separation. The efficiency of triplet formation is higher than 100%, and the disordered system leads to triplets living in the nanosecond time range.

查看原文本刊更多论文

水溶液中的过烯衍生物单色激子裂变

我们提供了水溶性化合物发生单子裂变的直接证据。我们的研究表明，过烯-3,4,9,10-四羧酸酯在水溶液中形成动态二聚体，其寿命长到足以发生单线裂变等分子间过程。由于这些是瞬时二聚体而不是稳定的聚集体，因此它们保留了很大程度的无序性。我们利用时间分辨吸收和荧光光谱学、核磁共振光谱学以及理论建模对这种动态组装体进行了全面分析，从而观察到了单子裂变的特征，并建立了一个模型来描述所观察到的不同物种。我们的研究结果表明，过烯烃-3,4,9,10-四羧酸酯结合体内部的结构波动是有利于单线裂变或电荷分离的关键。三重子的形成效率高于 100%，无序系统导致三重子在纳秒级的时间范围内存活。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

求助全文

约1分钟内获得全文求助全文

来源期刊

Chemical Science CHEMISTRY, MULTIDISCIPLINARY-

CiteScore

14.40

自引率

4.80%

发文量

1352

审稿时长

2.1 months

期刊介绍： Chemical Science is a journal that encompasses various disciplines within the chemical sciences. Its scope includes publishing ground-breaking research with significant implications for its respective field, as well as appealing to a wider audience in related areas. To be considered for publication, articles must showcase innovative and original advances in their field of study and be presented in a manner that is understandable to scientists from diverse backgrounds. However, the journal generally does not publish highly specialized research.