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Direct visualization of the charge transfer state dynamics in dilute-donor organic photovoltaic blends

Author

Listed:
  • Gareth John Moore

    (University of Bern)

  • Florian Günther

    (Universidade de São Paulo (USP)
    São Paulo State University (UNESP)
    Technische Universität)

  • Kaila M. Yallum

    (University of Bern)

  • Martina Causa’

    (University of Bern)

  • Anna Jungbluth

    (University of Oxford)

  • Julien Réhault

    (University of Bern)

  • Moritz Riede

    (University of Oxford)

  • Frank Ortmann

    (Technische Universität
    TUM School of Natural Sciences, Technische Universität München)

  • Natalie Banerji

    (University of Bern)

Abstract

The interconversion dynamics between charge transfer state charges (CTCs) and separated charges (SCs) is still an unresolved issue in the field of organic photovoltaics. Here, a transient absorption spectroscopy (TAS) study of a thermally evaporated small-molecule:fullerene system (α6T:C60) in different morphologies (dilute intermixed and phase separated) is presented. Spectral decomposition reveals two charge species with distinct absorption characteristics and different dynamics. Using time-dependent density functional theory, these species are identified as CTCs and SCs, where the spectral differences arise from broken symmetry in the charge transfer state that turns forbidden transitions into allowed ones. Based on this assignment, a kinetic model is formulated allowing the characterization of the charge generation, separation, and recombination mechanisms. We find that SCs are either formed directly from excitons within a few picoseconds or more slowly (~30–80 ps) from reversible splitting of CTCs. These findings constitute the first unambiguous observation of spectrally resolved CTCs and SCs.

Suggested Citation

  • Gareth John Moore & Florian Günther & Kaila M. Yallum & Martina Causa’ & Anna Jungbluth & Julien Réhault & Moritz Riede & Frank Ortmann & Natalie Banerji, 2024. "Direct visualization of the charge transfer state dynamics in dilute-donor organic photovoltaic blends," Nature Communications, Nature, vol. 15(1), pages 1-11, December.
    • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-53694-4
    DOI: 10.1038/s41467-024-53694-4
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