Ultra-fast intramolecular singlet fission to persistent multiexcitons by molecular design
View/ Open
s41557-019-0297-7.pdf (1.953Mb)
Access Status
Full text of the requested work is not available in DASH at this time ("restricted access"). For more information on restricted deposits, see our FAQ.Author
Pun, Andrew
Asadpoordarvish, Amir
Kumarasamy, Elango
Tayebjee, Murad
Niesner, Daniel
McCamey, Dane
Sanders, Samuel
Sfeir, Matthew
Campos, Luis
Published Version
https://doi.org/10.1038/s41557-019-0297-7Metadata
Show full item recordCitation
Pun, Andrew, Amir Asadpoordarvish, Murad Tayebjee, Daniel Niesner, Dane McCamey, Samuel Sanders, Luis Campos, and Matthew Sfeir. 2019. Ultra-fast Intramolecular Singlet Fission to Persistent Multiexcitons by Molecular Design. Nature Chemistry 11, no. 9: 821-28.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 ~20 µs.Citable link to this page
https://nrs.harvard.edu/URN-3:HUL.INSTREPOS:37374242
Collections
- FAS Scholarly Articles [18296]
Contact administrator regarding this item (to report mistakes or request changes)