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Direct observation of ultrafast exciton localization in an organic semiconductor with soft X-ray transient absorption spectroscopy

Author

Listed:
  • D. Garratt

    (Imperial College London)

  • L. Misiekis

    (Imperial College London)

  • D. Wood

    (Imperial College London)

  • E. W. Larsen

    (Imperial College London)

  • M. Matthews

    (Imperial College London)

  • O. Alexander

    (Imperial College London)

  • P. Ye

    (Imperial College London)

  • S. Jarosch

    (Imperial College London)

  • C. Ferchaud

    (Imperial College London)

  • C. Strüber

    (Imperial College London)

  • A. S. Johnson

    (Imperial College London)

  • A. A. Bakulin

    (Imperial College London)

  • T. J. Penfold

    (Newcastle University)

  • J. P. Marangos

    (Imperial College London)

Abstract

The localization dynamics of excitons in organic semiconductors influence the efficiency of charge transfer and separation in these materials. Here we apply time-resolved X-ray absorption spectroscopy to track photoinduced dynamics of a paradigmatic crystalline conjugated polymer: poly(3-hexylthiophene) (P3HT) commonly used in solar cell devices. The π→π* transition, the first step of solar energy conversion, is pumped with a 15 fs optical pulse and the dynamics are probed by an attosecond soft X-ray pulse at the carbon K-edge. We observe X-ray spectroscopic signatures of the initially hot excitonic state, indicating that it is delocalized over multiple polymer chains. This undergoes a rapid evolution on a sub 50 fs timescale which can be directly associated with cooling and localization to form either a localized exciton or polaron pair.

Suggested Citation

  • D. Garratt & L. Misiekis & D. Wood & E. W. Larsen & M. Matthews & O. Alexander & P. Ye & S. Jarosch & C. Ferchaud & C. Strüber & A. S. Johnson & A. A. Bakulin & T. J. Penfold & J. P. Marangos, 2022. "Direct observation of ultrafast exciton localization in an organic semiconductor with soft X-ray transient absorption spectroscopy," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-31008-w
    DOI: 10.1038/s41467-022-31008-w
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    References listed on IDEAS

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