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Vacancy control in acene blends links exothermic singlet fission to coherence

Author

Listed:
  • 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
    Northwestern University)

  • Katharina Broch

    (Institute of Applied Physics, University of Tübingen)

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.

Suggested Citation

  • Clemens Zeiser & Chad Cruz & David R. Reichman & Michael Seitz & Jan Hagenlocher & Eric L. Chronister & Christopher J. Bardeen & Roel Tempelaar & Katharina Broch, 2021. "Vacancy control in acene blends links exothermic singlet fission to coherence," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-25395-9
    DOI: 10.1038/s41467-021-25395-9
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