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 | |
| 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
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
}
TY - JOUR
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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U2 - 10.1038/ncomms15171
DO - 10.1038/ncomms15171
M3 - Article
VL - 8
JO - Nature Communications
JF - Nature Communications
SN - 2041-1723
M1 - 15171
ER -