Unified model for singlet fission within a non-conjugated covalent pentacene dimer

Bettina S. Basel; Johannes Zirzlmeier; Constantin Hetzer; Brian T. Phelan; Matthew D. Krzyaniak; S. Rajagopala Reddy; Pedro B. Coto; Noah E. Horwitz; Ryan M. Young; Fraser J. White; Frank Hampel; Timothy Clark; Michael Thoss; Rik R. Tykwinski; Michael R. Wasielewski; Dirk M. Guldi

doi:10.1038/ncomms15171

Unified model for singlet fission within a non-conjugated covalent pentacene dimer

Bettina S. Basel, Johannes Zirzlmeier, Constantin Hetzer, Brian T. Phelan, Matthew D. Krzyaniak, S. Rajagopala Reddy, Pedro B. Coto, Noah E. Horwitz, Ryan M. Young, Fraser J. White, Frank Hampel, Timothy Clark, Michael Thoss, Rik R. Tykwinski, Michael R. Wasielewski, Dirk M. Guldi^*

^*Corresponding author for this work

Research output: Contribution to journal › Article › peer-review

174 Scopus citations

Abstract

When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron-hole pairs, leading to a predicted 1/450% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state that precedes formation of the pentacene triplet excitons. Using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.

Original language	English (US)
Article number	15171
Journal	Nature communications
Volume	8
DOIs	https://doi.org/10.1038/ncomms15171
State	Published - May 18 2017

ASJC Scopus subject areas

General Chemistry
General Biochemistry, Genetics and Molecular Biology
General Physics and Astronomy

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10.1038/ncomms15171

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Basel, B. S., Zirzlmeier, J., Hetzer, C., Phelan, B. T., Krzyaniak, M. D., Reddy, S. R., Coto, P. B., Horwitz, N. E., Young, R. M., White, F. J., Hampel, F., Clark, T., Thoss, M., Tykwinski, R. R., Wasielewski, M. R., & Guldi, D. M. (2017). Unified model for singlet fission within a non-conjugated covalent pentacene dimer. Nature communications, 8, Article 15171. https://doi.org/10.1038/ncomms15171

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title = "Unified model for singlet fission within a non-conjugated covalent pentacene dimer",

abstract = "When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron-hole pairs, leading to a predicted 1/450% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state that precedes formation of the pentacene triplet excitons. Using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.",

author = "Basel, {Bettina S.} and Johannes Zirzlmeier and Constantin Hetzer and Phelan, {Brian T.} and Krzyaniak, {Matthew D.} and Reddy, {S. Rajagopala} and Coto, {Pedro B.} and Horwitz, {Noah E.} and Young, {Ryan M.} and White, {Fraser J.} and Frank Hampel and Timothy Clark and Michael Thoss and Tykwinski, {Rik R.} and Wasielewski, {Michael R.} and Guldi, {Dirk M.}",

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year = "2017",

month = may,

day = "18",

doi = "10.1038/ncomms15171",

language = "English (US)",

volume = "8",

journal = "Nature communications",

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T1 - Unified model for singlet fission within a non-conjugated covalent pentacene dimer

AU - Basel, Bettina S.

AU - Zirzlmeier, Johannes

AU - Hetzer, Constantin

AU - Phelan, Brian T.

AU - Krzyaniak, Matthew D.

AU - Reddy, S. Rajagopala

AU - Coto, Pedro B.

AU - Horwitz, Noah E.

AU - Young, Ryan M.

AU - White, Fraser J.

AU - Hampel, Frank

AU - Clark, Timothy

AU - Thoss, Michael

AU - Tykwinski, Rik R.

AU - Wasielewski, Michael R.

AU - Guldi, Dirk M.

PY - 2017/5/18

Y1 - 2017/5/18

N2 - When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron-hole pairs, leading to a predicted 1/450% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state that precedes formation of the pentacene triplet excitons. Using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.

AB - When molecular dimers, crystalline films or molecular aggregates absorb a photon to produce a singlet exciton, spin-allowed singlet fission may produce two triplet excitons that can be used to generate two electron-hole pairs, leading to a predicted 1/450% enhancement in maximum solar cell performance. The singlet fission mechanism is still not well understood. Here we report on the use of time-resolved optical and electron paramagnetic resonance spectroscopy to probe singlet fission in a pentacene dimer linked by a non-conjugated spacer. We observe the key intermediates in the singlet fission process, including the formation and decay of a quintet state that precedes formation of the pentacene triplet excitons. Using these combined data, we develop a single kinetic model that describes the data over seven temporal orders of magnitude both at room and cryogenic temperatures.

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JO - Nature communications

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Unified model for singlet fission within a non-conjugated covalent pentacene dimer

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CCDC 1503240: Experimental Crystal Structure Determination

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Unified model for singlet fission within a non-conjugated covalent pentacene dimer

Abstract

ASJC Scopus subject areas

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Datasets

CCDC 1503240: Experimental Crystal Structure Determination

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