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

Northwestern University

Research output: Contribution to journal › Article

80 Citations (Scopus)

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
Article number	15171
Journal	Nature Communications
Volume	8
DOIs	https://doi.org/10.1038/ncomms15171
Publication status	Published - May 18 2017

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ASJC Scopus subject areas

Chemistry(all)
Biochemistry, Genetics and Molecular Biology(all)
Physics and Astronomy(all)

Cite this

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, [15171]. https://doi.org/10.1038/ncomms15171

Unified model for singlet fission within a non-conjugated covalent pentacene dimer. / Basel, Bettina S.; Zirzlmeier, Johannes; Hetzer, Constantin; Phelan, Brian T.; Krzyaniak, Matthew D.; Reddy, S. Rajagopala; Coto, Pedro B.; Horwitz, Noah E.; Young, Ryan M.; White, Fraser J.; Hampel, Frank; Clark, Timothy; Thoss, Michael; Tykwinski, Rik R.; Wasielewski, Michael R; Guldi, Dirk M.

In: Nature Communications, Vol. 8, 15171, 18.05.2017.

Research output: Contribution to journal › Article

Basel, Bettina S. ; Zirzlmeier, Johannes ; Hetzer, Constantin ; Phelan, Brian T. ; Krzyaniak, Matthew D. ; Reddy, S. Rajagopala ; Coto, Pedro B. ; Horwitz, Noah E. ; Young, Ryan M. ; White, Fraser J. ; Hampel, Frank ; Clark, Timothy ; Thoss, Michael ; Tykwinski, Rik R. ; Wasielewski, Michael R ; Guldi, Dirk M. / Unified model for singlet fission within a non-conjugated covalent pentacene dimer. In: Nature Communications. 2017 ; Vol. 8.

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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.",

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AU - Basel, Bettina S.

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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

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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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10.1038/ncomms15171