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Tracking the coherent generation of polaron pairs in conjugated polymers

Author

Listed:
  • Antonietta De Sio

    (Institut für Physik, Carl von Ossietzky Universität
    Center of Interface Science, Carl von Ossietzky Universität)

  • Filippo Troiani

    (Istituto Nanoscienze—CNR)

  • Margherita Maiuri

    (IFN-CNR, Politecnico di Milano)

  • Julien Réhault

    (IFN-CNR, Politecnico di Milano)

  • Ephraim Sommer

    (Institut für Physik, Carl von Ossietzky Universität
    Center of Interface Science, Carl von Ossietzky Universität)

  • James Lim

    (Institut für Theoretische Physik and IQST, Universität Ulm)

  • Susana F. Huelga

    (Institut für Theoretische Physik and IQST, Universität Ulm)

  • Martin B. Plenio

    (Institut für Theoretische Physik and IQST, Universität Ulm)

  • Carlo Andrea Rozzi

    (Istituto Nanoscienze—CNR)

  • Giulio Cerullo

    (IFN-CNR, Politecnico di Milano)

  • Elisa Molinari

    (Istituto Nanoscienze—CNR
    Matematiche e Informatiche, Università di Modena e Reggio Emilia)

  • Christoph Lienau

    (Institut für Physik, Carl von Ossietzky Universität
    Center of Interface Science, Carl von Ossietzky Universität
    Research Center Neurosensory Science, Carl von Ossietzky Universität)

Abstract

The optical excitation of organic semiconductors not only generates charge-neutral electron-hole pairs (excitons), but also charge-separated polaron pairs with high yield. The microscopic mechanisms underlying this charge separation have been debated for many years. Here we use ultrafast two-dimensional electronic spectroscopy to study the dynamics of polaron pair formation in a prototypical polymer thin film on a sub-20-fs time scale. We observe multi-period peak oscillations persisting for up to about 1 ps as distinct signatures of vibronic quantum coherence at room temperature. The measured two-dimensional spectra show pronounced peak splittings revealing that the elementary optical excitations of this polymer are hybridized exciton-polaron-pairs, strongly coupled to a dominant underdamped vibrational mode. Coherent vibronic coupling induces ultrafast polaron pair formation, accelerates the charge separation dynamics and makes it insensitive to disorder. These findings open up new perspectives for tailoring light-to-current conversion in organic materials.

Suggested Citation

  • Antonietta De Sio & Filippo Troiani & Margherita Maiuri & Julien Réhault & Ephraim Sommer & James Lim & Susana F. Huelga & Martin B. Plenio & Carlo Andrea Rozzi & Giulio Cerullo & Elisa Molinari & Chr, 2016. "Tracking the coherent generation of polaron pairs in conjugated polymers," Nature Communications, Nature, vol. 7(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:7:y:2016:i:1:d:10.1038_ncomms13742
    DOI: 10.1038/ncomms13742
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    Cited by:

    1. Daniel Timmer & Moritz Gittinger & Thomas Quenzel & Sven Stephan & Yu Zhang & Marvin F. Schumacher & Arne Lützen & Martin Silies & Sergei Tretiak & Jin-Hui Zhong & Antonietta De Sio & Christoph Lienau, 2023. "Plasmon mediated coherent population oscillations in molecular aggregates," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
    2. Katia Pagano & Jin Gwan Kim & Joel Luke & Ellasia Tan & Katherine Stewart & Igor V. Sazanovich & Gabriel Karras & Hristo Ivov Gonev & Adam V. Marsh & Na Yeong Kim & Sooncheol Kwon & Young Yong Kim & M, 2024. "Slow vibrational relaxation drives ultrafast formation of photoexcited polaron pair states in glycolated conjugated polymers," Nature Communications, Nature, vol. 15(1), pages 1-13, December.
    3. 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.

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