Vacancy control in acene blends links exothermic singlet fission to coherence

Clemens Zeiser, Chad Cruz, David R. Reichman, Michael Seitz, Jan Hagenlocher, Eric L. Chronister, Christopher J. Bardeen, Roel Tempelaar () and Katharina Broch ()
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Clemens Zeiser: Institute of Applied Physics, University of Tübingen
Chad Cruz: University of California at Riverside
David R. Reichman: Columbia University
Michael Seitz: Institute of Inorganic Chemistry, University of Tübingen
Jan Hagenlocher: Institute of Applied Physics, University of Tübingen
Eric L. Chronister: University of Nevada, Las Vegas, 4505S. Maryland Pkwy
Christopher J. Bardeen: University of California at Riverside
Roel Tempelaar: Columbia University
Katharina Broch: Institute of Applied Physics, University of Tübingen

Nature Communications, 2021, vol. 12, issue 1, 1-9

Abstract: Abstract The fission of singlet excitons into triplet pairs in organic materials holds great technological promise, but the rational application of this phenomenon is hampered by a lack of understanding of its complex photophysics. Here, we use the controlled introduction of vacancies by means of spacer molecules in tetracene and pentacene thin films as a tuning parameter complementing experimental observables to identify the operating principles of different singlet fission pathways. Time-resolved spectroscopic measurements in combination with microscopic modelling enables us to demonstrate distinct scenarios, resulting from different singlet-to-triplet pair energy alignments. For pentacene, where fission is exothermic, coherent mixing between the photoexcited singlet and triplet-pair states is promoted by vibronic resonances, which drives the fission process with little sensitivity to the vacancy concentration. Such vibronic resonances do not occur for endothermic materials such as tetracene, for which we find fission to be fully incoherent; a process that is shown to slow down with increasing vacancy concentration.

Date: 2021
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DOI: 10.1038/s41467-021-25395-9

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