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Energy cascades in donor-acceptor exciton-polaritons observed by ultrafast two-dimensional white-light spectroscopy

Author

Listed:
  • Minjung Son

    (University of Wisconsin-Madison)

  • Zachary T. Armstrong

    (University of Wisconsin-Madison)

  • Ryan T. Allen

    (University of Wisconsin-Madison)

  • Abitha Dhavamani

    (University of Wisconsin-Madison)

  • Michael S. Arnold

    (University of Wisconsin-Madison)

  • Martin T. Zanni

    (University of Wisconsin-Madison)

Abstract

Exciton-polaritons are hybrid states formed when molecular excitons are strongly coupled to photons trapped in an optical cavity. These systems exhibit many interesting, but not fully understood, phenomena. Here, we utilize ultrafast two-dimensional white-light spectroscopy to study donor-acceptor microcavities made from two different layers of semiconducting carbon nanotubes. We observe the delayed growth of a cross peak between the upper- and lower-polariton bands that is oftentimes obscured by Rabi contraction. We simulate the spectra and use Redfield theory to learn that energy cascades down a manifold of new electronic states created by intermolecular coupling and the two distinct bandgaps of the donor and acceptor. Energy most effectively enters the manifold when light-matter coupling is commensurate with the energy distribution of the manifold, contributing to long-range energy transfer. Our results broaden the understanding of energy transfer dynamics in exciton-polariton systems and provide evidence that long-range energy transfer benefits from moderately-coupled cavities.

Suggested Citation

  • Minjung Son & Zachary T. Armstrong & Ryan T. Allen & Abitha Dhavamani & Michael S. Arnold & Martin T. Zanni, 2022. "Energy cascades in donor-acceptor exciton-polaritons observed by ultrafast two-dimensional white-light spectroscopy," Nature Communications, Nature, vol. 13(1), pages 1-10, December.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-35046-2
    DOI: 10.1038/s41467-022-35046-2
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    1. 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.
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    4. Andrea B. Grafton & Adam D. Dunkelberger & Blake S. Simpkins & Johan F. Triana & Federico J. Hernández & Felipe Herrera & Jeffrey C. Owrutsky, 2021. "Excited-state vibration-polariton transitions and dynamics in nitroprusside," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    5. Randy D. Mehlenbacher & Thomas J. McDonough & Maksim Grechko & Meng-Yin Wu & Michael S. Arnold & Martin T. Zanni, 2015. "Energy transfer pathways in semiconducting carbon nanotubes revealed using two-dimensional white-light spectroscopy," Nature Communications, Nature, vol. 6(1), pages 1-7, November.
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    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. Ilia Sokolovskii & Ruth H. Tichauer & Dmitry Morozov & Johannes Feist & Gerrit Groenhof, 2023. "Multi-scale molecular dynamics simulations of enhanced energy transfer in organic molecules under strong coupling," Nature Communications, Nature, vol. 14(1), pages 1-11, December.

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