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Direct observation of ultrafast singlet exciton fission in three dimensions

Author

Listed:
  • Arjun Ashoka

    (University of Cambridge)

  • Nicolas Gauriot

    (University of Cambridge)

  • Aswathy V. Girija

    (University of Cambridge)

  • Nipun Sawhney

    (University of Cambridge)

  • Alexander J. Sneyd

    (University of Cambridge)

  • Kenji Watanabe

    (National Institute for Materials Science)

  • Takashi Taniguchi

    (National Institute for Materials Science)

  • Jooyoung Sung

    (DGIST)

  • Christoph Schnedermann

    (University of Cambridge)

  • Akshay Rao

    (University of Cambridge)

Abstract

We present quantitative ultrafast interferometric pump-probe microscopy capable of tracking of photoexcitations with sub-10 nm spatial precision in three dimensions with 15 fs temporal resolution, through retrieval of the full transient photoinduced complex refractive index. We use this methodology to study the spatiotemporal dynamics of the quantum coherent photophysical process of ultrafast singlet exciton fission. Measurements on microcrystalline pentacene films grown on glass (SiO2) and boron nitride (hBN) reveal a 25 nm, 70 fs expansion of the joint-density-of-states along the crystal a,c-axes accompanied by a 6 nm, 115 fs change in the exciton density along the crystal b-axis. We propose that photogenerated singlet excitons expand along the direction of maximal orbital π-overlap in the crystal a,c-plane to form correlated triplet pairs, which subsequently electronically decouples into free triplets along the crystal b-axis due to molecular sliding motion of neighbouring pentacene molecules. Our methodology lays the foundation for the study of three dimensional transport on ultrafast timescales.

Suggested Citation

  • Arjun Ashoka & Nicolas Gauriot & Aswathy V. Girija & Nipun Sawhney & Alexander J. Sneyd & Kenji Watanabe & Takashi Taniguchi & Jooyoung Sung & Christoph Schnedermann & Akshay Rao, 2022. "Direct observation of ultrafast singlet exciton fission in three dimensions," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-33647-5
    DOI: 10.1038/s41467-022-33647-5
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    References listed on IDEAS

    as
    1. Samuele Giannini & Wei-Tao Peng & Lorenzo Cupellini & Daniele Padula & Antoine Carof & Jochen Blumberger, 2022. "Exciton transport in molecular organic semiconductors boosted by transient quantum delocalization," Nature Communications, Nature, vol. 13(1), pages 1-13, December.
    2. Arjun Ashoka & Ronnie R. Tamming & Aswathy V. Girija & Hope Bretscher & Sachin Dev Verma & Shang-Da Yang & Chih-Hsuan Lu & Justin M. Hodgkiss & David Ritchie & Chong Chen & Charles G. Smith & Christop, 2022. "Extracting quantitative dielectric properties from pump-probe spectroscopy," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    3. Raj Pandya & Richard Y. S. Chen & Qifei Gu & Jooyoung Sung & Christoph Schnedermann & Oluwafemi S. Ojambati & Rohit Chikkaraddy & Jeffrey Gorman & Gianni Jacucci & Olimpia D. Onelli & Tom Willhammar &, 2021. "Microcavity-like exciton-polaritons can be the primary photoexcitation in bare organic semiconductors," Nature Communications, Nature, vol. 12(1), pages 1-11, December.
    4. Shibin Deng & Enzheng Shi & Long Yuan & Linrui Jin & Letian Dou & Libai Huang, 2020. "Long-range exciton transport and slow annihilation in two-dimensional hybrid perovskites," Nature Communications, Nature, vol. 11(1), pages 1-8, December.
    5. Samuele Giannini & Antoine Carof & Matthew Ellis & Hui Yang & Orestis George Ziogos & Soumya Ghosh & Jochen Blumberger, 2019. "Quantum localization and delocalization of charge carriers in organic semiconducting crystals," Nature Communications, Nature, vol. 10(1), pages 1-12, December.
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