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Sub-picosecond collapse of molecular polaritons to pure molecular transition in plasmonic photoswitch-nanoantennas

Author

Listed:
  • Joel Kuttruff

    (University of Konstanz)

  • Marco Romanelli

    (University of Padova)

  • Esteban Pedrueza-Villalmanzo

    (University of Gothenburg
    Chalmers University of Technology)

  • Jonas Allerbeck

    (University of Konstanz
    nanotech@surfaces Laboratory, Empa, Swiss Federal Laboratories for Materials Science and Technology)

  • Jacopo Fregoni

    (Universidad Autónoma de Madrid, Ciudad Universitaria de Cantoblanco)

  • Valeria Saavedra-Becerril

    (Chalmers University of Technology)

  • Joakim Andréasson

    (Chalmers University of Technology)

  • Daniele Brida

    (University of Luxembourg)

  • Alexandre Dmitriev

    (University of Gothenburg)

  • Stefano Corni

    (University of Padova
    CNR Institute of Nanoscience)

  • Nicolò Maccaferri

    (University of Luxembourg
    Umeå University
    Umeå University)

Abstract

Molecular polaritons are hybrid light-matter states that emerge when a molecular transition strongly interacts with photons in a resonator. At optical frequencies, this interaction unlocks a way to explore and control new chemical phenomena at the nanoscale. Achieving such control at ultrafast timescales, however, is an outstanding challenge, as it requires a deep understanding of the dynamics of the collectively coupled molecular excitation and the light modes. Here, we investigate the dynamics of collective polariton states, realized by coupling molecular photoswitches to optically anisotropic plasmonic nanoantennas. Pump-probe experiments reveal an ultrafast collapse of polaritons to pure molecular transition triggered by femtosecond-pulse excitation at room temperature. Through a synergistic combination of experiments and quantum mechanical modelling, we show that the response of the system is governed by intramolecular dynamics, occurring one order of magnitude faster with respect to the uncoupled excited molecule relaxation to the ground state.

Suggested Citation

  • Joel Kuttruff & Marco Romanelli & Esteban Pedrueza-Villalmanzo & Jonas Allerbeck & Jacopo Fregoni & Valeria Saavedra-Becerril & Joakim Andréasson & Daniele Brida & Alexandre Dmitriev & Stefano Corni &, 2023. "Sub-picosecond collapse of molecular polaritons to pure molecular transition in plasmonic photoswitch-nanoantennas," Nature Communications, Nature, vol. 14(1), pages 1-10, December.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-39413-5
    DOI: 10.1038/s41467-023-39413-5
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    References listed on IDEAS

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    1. Dipak Samanta & Daria Galaktionova & Julius Gemen & Linda J. W. Shimon & Yael Diskin-Posner & Liat Avram & Petr Král & Rafal Klajn, 2018. "Publisher Correction: Reversible chromism of spiropyran in the cavity of a flexible coordination cage," Nature Communications, Nature, vol. 9(1), pages 1-2, December.
    2. Dipak Samanta & Daria Galaktionova & Julius Gemen & Linda J. W. Shimon & Yael Diskin-Posner & Liat Avram & Petr Král & Rafal Klajn, 2018. "Reversible chromism of spiropyran in the cavity of a flexible coordination cage," Nature Communications, Nature, vol. 9(1), pages 1-9, December.
    3. Rohit Chikkaraddy & Bart de Nijs & Felix Benz & Steven J. Barrow & Oren A. Scherman & Edina Rosta & Angela Demetriadou & Peter Fox & Ortwin Hess & Jeremy J. Baumberg, 2016. "Single-molecule strong coupling at room temperature in plasmonic nanocavities," Nature, Nature, vol. 535(7610), pages 127-130, July.
    4. Javier Galego & Francisco J. Garcia-Vidal & Johannes Feist, 2016. "Suppressing photochemical reactions with quantized light fields," Nature Communications, Nature, vol. 7(1), pages 1-6, December.
    5. Anton V. Zasedatelev & Anton V. Baranikov & Denis Sannikov & Darius Urbonas & Fabio Scafirimuto & Vladislav Yu. Shishkov & Evgeny S. Andrianov & Yurii E. Lozovik & Ullrich Scherf & Thilo Stöferle & Ra, 2021. "Publisher Correction: Single-photon nonlinearity at room temperature," Nature, Nature, vol. 600(7889), pages 19-19, December.
    6. D. Ballarini & M. De Giorgi & E. Cancellieri & R. Houdré & E. Giacobino & R. Cingolani & A. Bramati & G. Gigli & D. Sanvitto, 2013. "All-optical polariton transistor," Nature Communications, Nature, vol. 4(1), pages 1-8, June.
    7. Martín Caldarola & Pablo Albella & Emiliano Cortés & Mohsen Rahmani & Tyler Roschuk & Gustavo Grinblat & Rupert F. Oulton & Andrea V. Bragas & Stefan A. Maier, 2015. "Non-plasmonic nanoantennas for surface enhanced spectroscopies with ultra-low heat conversion," Nature Communications, Nature, vol. 6(1), pages 1-8, November.
    8. Satyendra Nath Gupta & Ora Bitton & Tomas Neuman & Ruben Esteban & Lev Chuntonov & Javier Aizpurua & Gilad Haran, 2021. "Complex plasmon-exciton dynamics revealed through quantum dot light emission in a nanocavity," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    9. Anton V. Zasedatelev & Anton V. Baranikov & Denis Sannikov & Darius Urbonas & Fabio Scafirimuto & Vladislav Yu. Shishkov & Evgeny S. Andrianov & Yurii E. Lozovik & Ullrich Scherf & Thilo Stöferle & Ra, 2021. "Single-photon nonlinearity at room temperature," Nature, Nature, vol. 597(7877), pages 493-497, September.
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