Ultra-fast intramolecular singlet fission to persistent multiexcitons by molecular design
Pun AB, Asadpoordarvish A, Kumarasamy E, Tayebjee MJY, Niesner D, Mccamey DR, Sanders SN, Campos LM, Sfeir MY (2019)
Publication Language: English
Publication Status: Published
Publication Type: Journal article
Publication year: 2019
Journal
Publisher: NATURE PUBLISHING GROUP
Book Volume: 11
Pages Range: 821-828
Journal Issue: 9
DOI: 10.1038/s41557-019-0297-7
Abstract
Singlet fission-that is, the generation of two triplets from a lone singlet state-has recently resurfaced as a promising process for the generation of multiexcitons in organic systems. Although advances in this area have led to the discovery of modular classes of chromophores, controlling the fate of the multiexciton states has been a major challenge; for example, promoting fast multiexciton generation while maintaining long triplet lifetimes. Unravelling the dynamical evolution of the spin- and energy conversion processes from the transition of singlet excitons to correlated triplet pairs and individual triplet excitons is necessary to design materials that are optimized for translational technologies. Here, we engineer molecules featuring a discrete energy gradient that promotes the migration of strongly coupled triplet pairs to a spatially separated, weakly coupled state that readily dissociates into free triplets. This 'energy cleft' concept allows us to combine the amplification and migration processes within a single molecule, with rapid dissociation of tightly bound triplet pairs into individual triplets that exhibit lifetimes of similar to 20 mu s.
Authors with CRIS profile
Involved external institutions
Columbia University
United States (USA) (US)
University of New South Wales (UNSW)
Australia (AU)
University of Cambridge
United Kingdom (GB)
Brookhaven National Laboratory
United States (USA) (US)
United States (USA) (US)
University of New South Wales (UNSW)
Australia (AU)
University of Cambridge
United Kingdom (GB)
Brookhaven National Laboratory
United States (USA) (US)
How to cite
APA:
Pun, A.B., Asadpoordarvish, A., Kumarasamy, E., Tayebjee, M.J.Y., Niesner, D., Mccamey, D.R.,... Sfeir, M.Y. (2019). Ultra-fast intramolecular singlet fission to persistent multiexcitons by molecular design. Nature Chemistry, 11(9), 821-828. https://dx.doi.org/10.1038/s41557-019-0297-7
MLA:
Pun, Andrew B., et al. "Ultra-fast intramolecular singlet fission to persistent multiexcitons by molecular design." Nature Chemistry 11.9 (2019): 821-828.
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