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Promoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers

Author

Listed:
  • Guiying He

    (City University of New York
    City University of New York)

  • Emily M. Churchill

    (Columbia University)

  • Kaia R. Parenti

    (Columbia University)

  • Jocelyn Zhang

    (Columbia University)

  • Pournima Narayanan

    (Stanford University
    Stanford University)

  • Faridah Namata

    (KTH Royal Institute of Technology, Department of Fibre and Polymer Technology)

  • Michael Malkoch

    (KTH Royal Institute of Technology, Department of Fibre and Polymer Technology)

  • Daniel N. Congreve

    (Stanford University)

  • Angelo Cacciuto

    (Columbia University)

  • Matthew Y. Sfeir

    (City University of New York
    City University of New York)

  • Luis M. Campos

    (Columbia University)

Abstract

Singlet fission and triplet-triplet annihilation upconversion are two multiexciton processes intimately related to the dynamic interaction between one high-lying energy singlet and two low-lying energy triplet excitons. Here, we introduce a series of dendritic macromolecules that serve as platform to study the effect of interchromophore interactions on the dynamics of multiexciton generation and decay as a function of dendrimer generation. The dendrimers (generations 1–4) consist of trimethylolpropane core and 2,2-bis(methylol)propionic acid (bis-MPA) dendrons that provide exponential growth of the branches, leading to a corona decorated with pentacenes for SF or anthracenes for TTA-UC. The findings reveal a trend where a few highly ordered sites emerge as the dendrimer generation grows, dominating the multiexciton dynamics, as deduced from optical spectra, and transient absorption spectroscopy. While the dendritic structures enhance TTA-UC at low annihilator concentrations in the largest dendrimers, the paired chromophore interactions induce a broadened and red-shifted excimer emission. In SF dendrimers of higher generations, the triplet dynamics become increasingly dominated by pairwise sites exhibiting strong coupling (Type II), which can be readily distinguished from sites with weaker coupling (Type I) by their spectral dynamics and decay kinetics.

Suggested Citation

  • Guiying He & Emily M. Churchill & Kaia R. Parenti & Jocelyn Zhang & Pournima Narayanan & Faridah Namata & Michael Malkoch & Daniel N. Congreve & Angelo Cacciuto & Matthew Y. Sfeir & Luis M. Campos, 2023. "Promoting multiexciton interactions in singlet fission and triplet fusion upconversion dendrimers," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-41818-1
    DOI: 10.1038/s41467-023-41818-1
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    References listed on IDEAS

    as
    1. Markus Einzinger & Tony Wu & Julia F. Kompalla & Hannah L. Smith & Collin F. Perkinson & Lea Nienhaus & Sarah Wieghold & Daniel N. Congreve & Antoine Kahn & Moungi G. Bawendi & Marc A. Baldo, 2019. "Sensitization of silicon by singlet exciton fission in tetracene," Nature, Nature, vol. 571(7763), pages 90-94, July.
    2. Benjamin D. Ravetz & Andrew B. Pun & Emily M. Churchill & Daniel N. Congreve & Tomislav Rovis & Luis M. Campos, 2019. "Author Correction: Photoredox catalysis using infrared light via triplet fusion upconversion," Nature, Nature, vol. 570(7759), pages 24-24, June.
    3. Benjamin D. Ravetz & Andrew B. Pun & Emily M. Churchill & Daniel N. Congreve & Tomislav Rovis & Luis M. Campos, 2019. "Photoredox catalysis using infrared light via triplet fusion upconversion," Nature, Nature, vol. 565(7739), pages 343-346, January.
    4. Daphné Lubert-Perquel & Enrico Salvadori & Matthew Dyson & Paul N. Stavrinou & Riccardo Montis & Hiroki Nagashima & Yasuhiro Kobori & Sandrine Heutz & Christopher W. M. Kay, 2018. "Identifying triplet pathways in dilute pentacene films," Nature Communications, Nature, vol. 9(1), pages 1-10, December.
    5. Snellenburg, Joris J. & Laptenok, Sergey & Seger, Ralf & Mullen, Katharine M. & van Stokkum, Ivo H. M., 2012. "Glotaran: A Java-Based Graphical User Interface for the R Package TIMP," Journal of Statistical Software, Foundation for Open Access Statistics, vol. 49(i03).
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