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Plasmon mediated coherent population oscillations in molecular aggregates

Author

Listed:
  • Daniel Timmer

    (Carl von Ossietzky Universität)

  • Moritz Gittinger

    (Carl von Ossietzky Universität)

  • Thomas Quenzel

    (Carl von Ossietzky Universität)

  • Sven Stephan

    (Carl von Ossietzky Universität
    University of Applied Sciences)

  • Yu Zhang

    (Theoretical Division, Los Alamos National Laboratory)

  • Marvin F. Schumacher

    (University of Bonn)

  • Arne Lützen

    (University of Bonn)

  • Martin Silies

    (Carl von Ossietzky Universität
    University of Applied Sciences)

  • Sergei Tretiak

    (Theoretical Division, Los Alamos National Laboratory)

  • Jin-Hui Zhong

    (Carl von Ossietzky Universität
    Southern University of Science and Technology)

  • Antonietta De Sio

    (Carl von Ossietzky Universität
    Carl von Ossietzky Universität)

  • Christoph Lienau

    (Carl von Ossietzky Universität
    Carl von Ossietzky Universität
    Carl von Ossietzky Universität)

Abstract

The strong coherent coupling of quantum emitters to vacuum fluctuations of the light field offers opportunities for manipulating the optical and transport properties of nanomaterials, with potential applications ranging from ultrasensitive all-optical switching to creating polariton condensates. Often, ubiquitous decoherence processes at ambient conditions limit these couplings to such short time scales that the quantum dynamics of the interacting system remains elusive. Prominent examples are strongly coupled exciton-plasmon systems, which, so far, have mostly been investigated by linear optical spectroscopy. Here, we use ultrafast two-dimensional electronic spectroscopy to probe the quantum dynamics of J-aggregate excitons collectively coupled to the spatially structured plasmonic fields of a gold nanoslit array. We observe rich coherent Rabi oscillation dynamics reflecting a plasmon-driven coherent exciton population transfer over mesoscopic distances at room temperature. This opens up new opportunities to manipulate the coherent transport of matter excitations by coupling to vacuum fields.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-43578-4
    DOI: 10.1038/s41467-023-43578-4
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