Spin Dynamics of Quintet and Triplet States Resulting from Singlet Fission in Oriented Terrylenediimide and Quaterrylenediimide Films

Youn Jue Bae, Xingang Zhao, Matthew D. Kryzaniak, Hiroki Nagashima, Joseph Strzalka, Qingteng Zhang, Michael R. Wasielewski

Research output: Contribution to journalArticlepeer-review

Abstract

Singlet fission in organic semiconductors provides an important opportunity to study high-spin states in electronically coupled chromophores. Photoexcitation of oriented, crystalline films of N,N-bis(pentadec-8-yl)terrylene-3,4:11,12-bis(dicarboximide) (TDI) and N,N-bis(pentadec-8-yl)quaterrylene-3,4:13,14-bis(dicarboximide) (QDI) result in the formation of the correlated triplet pair quintet state, 5(T1T1) and its subsequent dissociation into two triplet (T1) excitons. Time-resolved electron paramagnetic resonance (TREPR) spectroscopy and X-ray crystallography are used to show that the orientation dependence of 5(T1T1) spin dynamics is retained as it dissociates into two T1 excitons, while such information is lost in a randomly oriented sample. In addition, the spin dynamics depend on how the molecules are oriented relative to the external applied magnetic field. Dissociation of 5(T1T1) to form two T1 excitons is more efficient in TDI and leads to a longer T1 lifetime than in QDI, making TDI a more viable candidate for photovoltaic applications. Since QDI readily forms a highly oriented film, and the lifetime of its 5(T1T1) state is longer than that of TDI, it may be a good candidate for quantum information science applications that require the generation of a quantum-entangled, four-spin state.

Original languageEnglish
Pages (from-to)9822-9833
Number of pages12
JournalJournal of Physical Chemistry C
Volume124
Issue number18
DOIs
Publication statusPublished - May 7 2020

ASJC Scopus subject areas

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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