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

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

doi:10.1021/acs.jpcc.0c03189

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

Journal Article · Tue Apr 14 00:00:00 EDT 2020 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.0c03189· OSTI ID:1635107

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Northwestern Univ., Evanston, IL (United States)
Saitama Univ. (Japan)
Argonne National Lab. (ANL), Argonne, IL (United States)

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 (T-1) 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 T-1 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.

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Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1635107

Journal Information:: Journal of Physical Chemistry. C, Vol. 124, Issue 18; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 12 works

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