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Modulating Singlet Fission by Scanning through Vibronic Resonances in Pentacene-Based Blends

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    Modulating Singlet Fission by Scanning through Vibronic Resonances in Pentacene-Based Blends
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2022, 144, 45, 20610–20619
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    https://doi.org/10.1021/jacs.2c07237
    Published November 1, 2022
    Copyright © 2022 American Chemical Society
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    Abstract

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    Vibronic coupling has been proposed to play a decisive role in promoting ultrafast singlet fission (SF), the conversion of a singlet exciton into two triplet excitons. Its inherent complexity is challenging to explore, both from a theoretical and an experimental point of view, due to the variety of potentially relevant vibrational modes. Here, we report a study on blends of the prototypical SF chromophore pentacene in which we engineer the polarizability of the molecular environment to scan the energy of the excited singlet state (S1) continuously over a narrow energy range, covering vibrational sublevels of the triplet-pair state (1(TT)). Using femtosecond transient absorption spectroscopy, we probe the dependence of the SF rate on energetic resonance between vibronic states and, by comparison with simulation, identify vibrational modes near 1150 cm–1 as key in facilitating ultrafast SF in pentacene.

    Copyright © 2022 American Chemical Society

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    Supporting Information

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/jacs.2c07237.

    • Details on experimental methods; details on structural analysis including X-ray reflectivity and grazing incidence wide-angle X-ray scattering data, probability for the number of nearest neighbors in the blends, UV–vis absorption spectra and analysis, temperature-dependent photoluminescence spectra, transient absorption data and analysis; and details on the simulations (PDF)

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    Cited By

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    This article is cited by 5 publications.

    1. Marina Gerhard, Julian Hausch, Nico Hofeditz, Jona Bredehöft, Katharina Broch, Frank Schreiber. Singlet Fission in a Binary System: Effect of Structural Changes and Temperature. The Journal of Physical Chemistry C 2024, 128 (33) , 13926-13936. https://doi.org/10.1021/acs.jpcc.4c03155
    2. Frederik Unger, Daniel Lepple, Maximilian Asbach, Luca Craciunescu, Clemens Zeiser, Andreas F. Kandolf, Zbyněk Fišer, Jakub Hagara, Jan Hagenlocher, Stefan Hiller, Sara Haug, Marian Deutsch, Peter Grüninger, Jiří Novák, Holger F. Bettinger, Katharina Broch, Bernd Engels, Frank Schreiber. Optical Absorption Properties in Pentacene/Tetracene Solid Solutions. The Journal of Physical Chemistry A 2024, 128 (4) , 747-760. https://doi.org/10.1021/acs.jpca.3c06737
    3. Peter A. Rose, Jacob J. Krich. Interpretations of High-Order Transient Absorption Spectroscopies. The Journal of Physical Chemistry Letters 2023, 14 (48) , 10849-10855. https://doi.org/10.1021/acs.jpclett.3c02491
    4. Julian Hausch, Nico Hofeditz, Jona Bredehöft, Sebastian Hammer, Jens Pflaum, Katharina Broch, Marina Gerhard, Frank Schreiber. Influence of Excited-State Delocalization on Singlet Fission: Tuning Triplet-Pair-State Emission in Thin Films. The Journal of Physical Chemistry C 2023, 127 (7) , 3778-3786. https://doi.org/10.1021/acs.jpcc.2c08334
    5. Yiting Bai, Wenjun Ni, Kewei Sun, Lipeng Chen, Lin Ma, Yang Zhao, Gagik G. Gurzadyan, Maxim F. Gelin. Plenty of Room on the Top: Pathways and Spectroscopic Signatures of Singlet Fission from Upper Singlet States. The Journal of Physical Chemistry Letters 2022, 13 (48) , 11086-11094. https://doi.org/10.1021/acs.jpclett.2c03053
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    Journal of the American Chemical Society

    Cite this: J. Am. Chem. Soc. 2022, 144, 45, 20610–20619
    Click to copy citationCitation copied!
    https://doi.org/10.1021/jacs.2c07237
    Published November 1, 2022
    Copyright © 2022 American Chemical Society
    Request reuse permissions

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