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极化激元与分子陷阱态之间的相互作用。

Interplay between Polaritonic and Molecular Trap States.

作者信息

Mony Jürgen, Yu Yi, Schäfer Clara, Mallick Suman, Kushwaha Khushbu, Börjesson Karl

机构信息

Department of Chemistry and Molecular Biology, University of Gothenburg, Kemigården 4, Gothenburg 41296, Sweden.

出版信息

J Phys Chem C Nanomater Interfaces. 2022 May 12;126(18):7965-7972. doi: 10.1021/acs.jpcc.2c01239. Epub 2022 May 3.

DOI:10.1021/acs.jpcc.2c01239
PMID:35592736
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9109220/
Abstract

Strong exciton-photon coupling exhibits the possibility to modify the photophysical properties of organic molecules. This is due to the introduction of hybrid light-matter states, called polaritons, which have unique physical and optical properties. Those strongly coupled systems provide altered excited-state dynamics in comparison to the bare molecule case. In this study, we investigate the interplay between polaritonic and molecular trap states, such as excimers. The molecules used in this study show either prompt or delayed emission from trap states. For both cases, a clear dependency on the exciton-photon energy tuning was observed. Polaritonic emission gradually increased with a concurrent removal of aggregation-induced emission when the systems were tuned toward lower energies. For prompt emission, it is not clear whether the experimental results are best explained by a predominant relaxation toward the lower polariton after excitation or by a direct excimer to polariton transition. However, for the delayed emission case, trap states are formed on the initially formed triplet manifold, making it evident that an excimer-to-polariton transition has occurred. These results unveil the possibility to control the trap state population by creating a strongly coupled system, which may form a mitigation strategy to counteract detrimental trap states in photonic applications.

摘要

强激子 - 光子耦合展现出改变有机分子光物理性质的可能性。这是由于引入了称为极化激元的混合光 - 物质态,其具有独特的物理和光学性质。与裸分子情况相比,那些强耦合系统提供了改变的激发态动力学。在本研究中,我们研究极化激元态与分子陷阱态(如激基缔合物)之间的相互作用。本研究中使用的分子显示出从陷阱态的即时或延迟发射。对于这两种情况,均观察到对激子 - 光子能量调谐的明显依赖性。当系统调谐至较低能量时,极化激元发射逐渐增加,同时聚集诱导发射被消除。对于即时发射,尚不清楚实验结果是最好由激发后向较低极化激元的主要弛豫来解释,还是由直接的激基缔合物到极化激元的转变来解释。然而,对于延迟发射情况,陷阱态在最初形成的三重态流形上形成,这表明明显发生了激基缔合物到极化激元的转变。这些结果揭示了通过创建强耦合系统来控制陷阱态数量的可能性,这可能形成一种缓解策略,以应对光子应用中有害的陷阱态。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/8a3d4e006128/jp2c01239_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/97fa62467719/jp2c01239_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/2d5b1b6237f5/jp2c01239_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/53e380a8b77b/jp2c01239_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/8a3d4e006128/jp2c01239_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/97fa62467719/jp2c01239_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/2d5b1b6237f5/jp2c01239_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/53e380a8b77b/jp2c01239_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/25de/9109220/8a3d4e006128/jp2c01239_0005.jpg

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本文引用的文献

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Nat Commun. 2021 May 31;12(1):3255. doi: 10.1038/s41467-021-23481-6.
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Direct Transition from Triplet Excitons to Hybrid Light-Matter States via Triplet-Triplet Annihilation.通过三重态-三重态湮灭实现三重态激子向混合光-物质态的直接转变。
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Effect of molecular Stokes shift on polariton dynamics.分子斯托克斯位移对极化激元动力学的影响。
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Polariton-assisted excitation energy channeling in organic heterojunctions.有机异质结中的极化激元辅助激发能量通道化
Nat Commun. 2021 Mar 25;12(1):1874. doi: 10.1038/s41467-021-22183-3.
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Entropic Mixing Allows Monomeric-Like Absorption in Neat BODIPY Films.熵混合允许在纯净的 BODIPY 薄膜中具有单体样的吸收。
Chemistry. 2020 Nov 11;26(63):14295-14299. doi: 10.1002/chem.202002463. Epub 2020 Oct 1.
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Manipulating molecules with strong coupling: harvesting triplet excitons in organic exciton microcavities.利用强耦合操控分子:在有机激子微腔中捕获三重态激子。
Chem Sci. 2019 Nov 27;11(2):343-354. doi: 10.1039/c9sc04950a. eCollection 2020 Jan 14.
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Optimizing photon upconversion by decoupling excimer formation and triplet triplet annihilation.通过解耦激基复合物形成和三重态-三重态湮灭来优化光子上转换。
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