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Bae, Youn Jue; Shimizu, Daiki; Schultz, Jonathan D; Kang, Gyeongwon; Zhou, Jiawang; Schatz, George C; Osuka, Atsuhiro; Wasielewski, Michael R
The journal of physical chemistry. A, Molecules, spectroscopy, kinetics, environment, & general theory, 10/2020, Letnik: 124, Številka: 41Journal Article
Photoexcitation of molecular chromophore aggregates can form excimer states that play a significant role in photophysical processes such as charge and energy transfer as well as singlet fission. An excimer state is commonly defined as a superposition of Frenkel exciton and charge transfer states. In this work, we investigate the dynamics of excimer formation and decay in π-stacked 9,10-bis(phenylethynyl)anthracene (BPEA) covalent dimers appended to a xanthene spacer, where the electronic coupling between the two BPEA molecules is adjusted by changing their longitudinal molecular slip distances. Using exciton coupling calculations, we quantify the relative contributions of Frenkel excitons and charge transfer states and find that there is an upper and lower threshold of the charge transfer contribution for efficient excimer formation to occur. Knowing these thresholds can aid the design of molecular aggregates that optimize singlet fission.
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