Controlling Long-Lived Triplet Generation from Intramolecular Singlet Fission in the Solid State

Pace, Natalie A.; Zhang, Weimin; Arias, Dylan H.; McCulloch, Iain; Rumbles, Garry; Johnson, Justin C.

doi:10.1021/acs.jpclett.7b02750

Controlling Long-Lived Triplet Generation from Intramolecular Singlet Fission in the Solid State

Journal Article · Wed Nov 29 23:00:00 EST 2017 · Journal of Physical Chemistry Letters

DOI:https://doi.org/10.1021/acs.jpclett.7b02750· OSTI ID:1413905

^[1]; Zhang, Weimin ^[2]; ^[3]; ^[4]; Rumbles, Garry ^[1]; ^[3]

National Renewable Energy Lab. (NREL), Golden, CO (United States); Univ. of Colorado, Boulder, CO (United States)
Imperial College, London (United Kingdom)
National Renewable Energy Lab. (NREL), Golden, CO (United States)
Imperial College, London (United Kingdom); King Abdullah Univ. of Science and Technology, Thuwal (Saudi Arabia)

The conjugated polymer poly(benzothiophene dioxide) (PBTDO1) has recently been shown to exhibit efficient intramolecular singlet fission in solution. We investigate the role of intermolecular interactions in triplet separation dynamics after singlet fission. We use transient absorption spectroscopy to determine the singlet fission rate and triplet yield in two polymers differing only by side-chain motif in both solution and the solid state. Whereas solid-state films show singlet fission rates identical to those measured in solution, the average lifetime of the triplet population increases dramatically and is strongly dependent on side-chain identity. These results show that it may be necessary to carefully engineer the solid-state microstructure of these 'singlet fission polymers' to produce the long-lived triplets needed to realize efficient photovoltaic devices.

View Accepted Manuscript (DOE)

Research Organization:: National Renewable Energy Lab. (NREL), Golden, CO (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC36-08GO28308

OSTI ID:: 1413905

Report Number(s):: NREL/JA--5900-70338

Journal Information:: Journal of Physical Chemistry Letters, Journal Name: Journal of Physical Chemistry Letters Journal Issue: 24 Vol. 8; ISSN 1948-7185

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited By (9)

Dynamics of singlet fission and electron injection in self-assembled acene monolayers on titanium dioxide Pace, Natalie A.; Arias, Dylan H.; Granger, Devin B. Chemical Science, Vol. 9, Issue 11 https://doi.org/10.1039/c7sc04688j	journal	January 2018
Solution-Processable, Solid State Donor-Acceptor Materials for Singlet Fission Masoomi-Godarzi, Saghar; Liu, Maning; Tachibana, Yasuhiro Advanced Energy Materials, Vol. 8, Issue 30 https://doi.org/10.1002/aenm.201801720	journal	September 2018
Efficient triplet pair separation from intramolecular singlet fission in dibenzopentalene derivatives Liu, Yanping; Wu, Yishi; Wang, Long Science China Chemistry, Vol. 62, Issue 8 https://doi.org/10.1007/s11426-019-9482-y	journal	May 2019
Sensitizer-free photon up conversion in (HQ) ₂ ZnCl ₄ and HQCl crystals: systems involving resonant energy transfer and triplet–triplet annihilation Samet, Amira; Pillet, Sebastien; Abid, Younes Physical Chemistry Chemical Physics, Vol. 22, Issue 3 https://doi.org/10.1039/c9cp04435c	journal	January 2020
Morphology independent triplet formation in pentalene films: Singlet fission as the triplet formation mechanism Wang, Long; Wu, Yishi; Liu, Yanping The Journal of Chemical Physics, Vol. 151, Issue 12 https://doi.org/10.1063/1.5097192	journal	September 2019
Resolving population dynamics and interactions of multiple triplet excitons one molecule at a time Datko, Benjamin D.; Grimm, Ryan; Walwark, David J. The Journal of Chemical Physics, Vol. 151, Issue 4 https://doi.org/10.1063/1.5099920	journal	July 2019
Vibronic fingerprint of singlet fission in hexacene Deng, Gang-Hua; Wei, Qianshun; Han, Jian The Journal of Chemical Physics, Vol. 151, Issue 5 https://doi.org/10.1063/1.5110263	journal	August 2019
Heavy-atom effects on intramolecular singlet fission in a conjugated polymer Musser, Andrew J.; Al-Hashimi, Mohammed; Heeney, Martin The Journal of Chemical Physics, Vol. 151, Issue 4 https://doi.org/10.1063/1.5110269	journal	July 2019
Lessons from intramolecular singlet fission with covalently bound chromophores Korovina, Nadezhda V.; Pompetti, Nicholas F.; Johnson, Justin C. The Journal of Chemical Physics, Vol. 152, Issue 4 https://doi.org/10.1063/1.5135307	journal	January 2020

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
intermolecular interactions
separation dynamics
singlet fission
solid-state microstructure

Controlling Long-Lived Triplet Generation from Intramolecular Singlet Fission in the Solid State

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