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Direct observation of ultrafast long-range charge separation at polymer–fullerene heterojunctions

Author

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  • Françoise Provencher

    (Université de Montréal, C.P. 6128, Succursale Centre-Ville)

  • Nicolas Bérubé

    (Université de Montréal, C.P. 6128, Succursale Centre-Ville)

  • Anthony W. Parker

    (Central Laser Facility, Research Complex at Harwell, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Harwell Oxford)

  • Gregory M. Greetham

    (Central Laser Facility, Research Complex at Harwell, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Harwell Oxford)

  • Michael Towrie

    (Central Laser Facility, Research Complex at Harwell, Science and Technology Facilities Council, Rutherford Appleton Laboratory, Harwell Oxford)

  • Christoph Hellmann

    (Centre for Plastic Electronics, Imperial College London, South Kensington Campus)

  • Michel Côté

    (Université de Montréal, C.P. 6128, Succursale Centre-Ville)

  • Natalie Stingelin

    (Centre for Plastic Electronics, Imperial College London, South Kensington Campus)

  • Carlos Silva

    (Université de Montréal, C.P. 6128, Succursale Centre-Ville
    Imperial College London, South Kensington Campus)

  • Sophia C. Hayes

    (University of Cyprus, P.O. Box 20537)

Abstract

In polymeric semiconductors, charge carriers are polarons, which means that the excess charge deforms the molecular structure of the polymer chain that hosts it. This results in distinctive signatures in the vibrational modes of the polymer. Here, we probe polaron photogeneration dynamics at polymer:fullerene heterojunctions by monitoring its time-resolved resonance-Raman spectrum following ultrafast photoexcitation. We conclude that polarons emerge within 300 fs. Surprisingly, further structural evolution on ≲50-ps timescales is modest, indicating that the polymer conformation hosting nascent polarons is not significantly different from that near equilibrium. We interpret this as suggestive that charges are free from their mutual Coulomb potential because we would expect rich vibrational dynamics associated with charge-pair relaxation. We address current debates on the photocarrier generation mechanism at molecular heterojunctions, and our work is, to our knowledge, the first direct probe of molecular conformation dynamics during this fundamentally important process in these materials.

Suggested Citation

  • Françoise Provencher & Nicolas Bérubé & Anthony W. Parker & Gregory M. Greetham & Michael Towrie & Christoph Hellmann & Michel Côté & Natalie Stingelin & Carlos Silva & Sophia C. Hayes, 2014. "Direct observation of ultrafast long-range charge separation at polymer–fullerene heterojunctions," Nature Communications, Nature, vol. 5(1), pages 1-11, September.
    • Handle: RePEc:nat:natcom:v:5:y:2014:i:1:d:10.1038_ncomms5288
    DOI: 10.1038/ncomms5288
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    Cited by:

    1. Marios Maimaris & Allan J. Pettipher & Mohammed Azzouzi & Daniel J. Walke & Xijia Zheng & Andrei Gorodetsky & Yifan Dong & Pabitra Shakya Tuladhar & Helder Crespo & Jenny Nelson & John W. G. Tisch & A, 2022. "Sub-10-fs observation of bound exciton formation in organic optoelectronic devices," Nature Communications, Nature, vol. 13(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. 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.

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