Two Birds with One Stone: Tailoring Singlet Fission for Both Triplet Yield and Exciton Diffusion Length

Zhu, Tong; Wan, Yan; Guo, Zhi; Johnson, Justin C.; Huang, Libai

doi:10.1002/adma.201600968

Cited by 79 publications

(153 citation statements)

References 46 publications

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“…(ω T T > ω e ) so that k SF k T F and the TT population decays to zero for long t. The experimental TT yield of tetracene is well above zero [29,30], which is in contrast with our findings (see Fig. 2).…”

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confidence: 99%

Polariton-Assisted Singlet Fission in Acene Aggregates

Martínez-Martínez

Ribeiro

et al. 2018

J. Phys. Chem. Lett.

126

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Singlet fission is an important candidate to increase energy conversion efficiency in organic photovoltaics by providing a pathway to increase the quantum yield of excitons per photon absorbed in select materials. We investigate the dependence of exciton quantum yield for acenes in the strong light-matter interaction (polariton) regime, where the materials are embedded in optical microcavities. Starting from an open-quantum-systems approach, we build a kinetic model for time-evolution of species of interest in the presence of singlet quenchers and show that polaritons can decrease or increase exciton quantum yields compared to the cavity-free case. In particular, we find that hexacene, under the conditions of our model, can feature a higher yield than cavity-free pentacene when assisted by polaritonic effects. Similarly, we show that pentacene yield can be increased when assisted by polariton states. Finally, we address how various relaxation processes between bright and dark states in lossy microcavities affect polariton photochemistry. Our results also provide insights on how to choose microcavities to enhance similarly related chemical processes.

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contrasting

confidence: 99%

Polariton-Assisted Singlet Fission in Acene Aggregates

Martínez-Martínez

Ribeiro

et al. 2018

J. Phys. Chem. Lett.

126

140

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“…[80][81][82][83] As shown in Fig. 4, the spatial spread of the signal at each delay time can be fitted with a Gaussian function parameterized by variance s. The exciton diffusion length L at delay time t is then related to the exciton density characterized by variance s,…”

Section: (5) Direct Visualization Of Tetmentioning

confidence: 99%

Triplet transport in thin films: fundamentals and applications

Tang

2017

Chem. Commun.

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Triplet excitons are key players in multi-excitonic processes like singlet fission and triplet-triplet annihilation based photon upconversion, which may be useful in next-generation photovoltaic devices, photocatalysis and bioimaging. Here, we present an overview of experimental and theoretical work on triplet energy transfer, with a focus on triplet transport in thin films. We start with the theory describing Dexter-mediated triplet energy transfer and the fundamental parameters controlling this process. Then we summarize current experimental methods used to measure the triplet exciton diffusion length. Finally, the use of hierarchically ordered structures to improve the triplet diffusion length is presented, before concluding with an outlook on the remaining challenges.

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“…In addition, there have been several studies of exciton transport in polyacene single crystals of interest to singlet ssion. [38][39][40] However, studies that employ transient optical absorption measurements to study CT exciton dynamics in single D-A co-crystals are relatively rare. In one of the rst examples, Port and co-workers reported on the ultrafast CT exciton dynamics in single crystals of anthracene and PMDA, where they observed transient spectral features that they attributed to a Stark effect of the CT exciton on the absorption spectra of nearby molecules.…”

Section: Introductionmentioning

confidence: 99%