Enabling singlet fission by controlling intramolecular charge transfer in π-stacked covalent terrylenediimide dimers

Eric A. Margulies, Claire E. Miller, Yilei Wu, Lin Ma, George C Schatz, Ryan M. Young, Michael R Wasielewski

Research output: Contribution to journalArticle

82 Citations (Scopus)

Abstract

When an assembly of two or more molecules absorbs a photon to form a singlet exciton, and the energetics and intermolecular interactions are favourable, the singlet exciton can rapidly and spontaneously produce two triplet excitons by singlet fission. To understand this process is important because it may prove to be technologically significant for enhancing solar-cell performance. Theory strongly suggests that charge-transfer states are involved in singlet fission, but their role has remained an intriguing puzzle and, up until now, no molecular system has provided clear evidence for such a state. Here we describe a terrylenediimide dimer that forms a charge-transfer state in a few picoseconds in polar solvents, and undergoes equally rapid, high-yield singlet fission in nonpolar solvents. These results show that adjusting the charge-transfer-state energy relative to those of the exciton states can serve to either inhibit or promote singlet fission.

Original languageEnglish
Pages (from-to)1120-1125
Number of pages6
JournalNature Chemistry
Volume8
Issue number12
DOIs
Publication statusPublished - Dec 1 2016

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Excitons
Dimers
Charge transfer
Electron energy levels
Solar cells
Photons
Molecules
LDS 751

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

Cite this

Enabling singlet fission by controlling intramolecular charge transfer in π-stacked covalent terrylenediimide dimers. / Margulies, Eric A.; Miller, Claire E.; Wu, Yilei; Ma, Lin; Schatz, George C; Young, Ryan M.; Wasielewski, Michael R.

In: Nature Chemistry, Vol. 8, No. 12, 01.12.2016, p. 1120-1125.

Research output: Contribution to journalArticle

Margulies, Eric A. ; Miller, Claire E. ; Wu, Yilei ; Ma, Lin ; Schatz, George C ; Young, Ryan M. ; Wasielewski, Michael R. / Enabling singlet fission by controlling intramolecular charge transfer in π-stacked covalent terrylenediimide dimers. In: Nature Chemistry. 2016 ; Vol. 8, No. 12. pp. 1120-1125.
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