Journal
NATURE PHYSICS
Volume 13, Issue 2, Pages 182-188Publisher
NATURE PUBLISHING GROUP
DOI: 10.1038/NPHYS3909
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Funding
- Australian Research Council [DP160103008, LE130100146]
- ARENA Fellowship
- CASS Foundation
- ARC Future Fellowship [FT130100214]
- Office of Naval Research [N00014-15-1-2532]
- US DOE Office of Science [DE-SC0012704]
- Australian Research Council [LE130100146] Funding Source: Australian Research Council
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Singlet fission, in which two triplet excitons are generated from a single absorbed photon, is a key third -generation solar cell concept. Conservation of angular momentum requires that singlet fission populates correlated multiexciton states, which can subsequently dissociate to generate free triplets. However, little is known about electronic and spin correlations in these systems since, due to its typically short lifetime, the multiexciton state is challenging to isolate and study. Here, we use bridged pentacene dimers, which undergo intramolecular singlet fission while isolated in solution and in solid matrices, as a unimolecular model system that can trap long-lived multiexciton states. We combine transient absorption and time resolved electron spin resonance spectroscopies to show that spin correlations in the multiexciton state persist for hundreds of nanoseconds. Furthermore, we confirm long-standing predictions that singlet fission produces triplet pair states of quintet character. We compare two different pentacene-bridge-pentacene chromophores, systematically tuning the coupling between the pentacenes to understand how differences in molecular structure affect the population and dissociation of multiexciton quintet states.
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