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Coherent coupling of molecular resonators with a microcavity mode

Author

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  • A. Shalabney

    (ISIS & icFRC, University of Strasbourg and CNRS (UMR 7006))

  • J. George

    (ISIS & icFRC, University of Strasbourg and CNRS (UMR 7006))

  • J. Hutchison

    (ISIS & icFRC, University of Strasbourg and CNRS (UMR 7006))

  • G. Pupillo

    (IPCMS (UMR 7504) & ISIS (UMR 7006), University of Strasbourg and CNRS (UMR 7006))

  • C. Genet

    (ISIS & icFRC, University of Strasbourg and CNRS (UMR 7006))

  • T. W. Ebbesen

    (ISIS & icFRC, University of Strasbourg and CNRS (UMR 7006))

Abstract

The optical hybridization of the electronic states in strongly coupled molecule–cavity systems have revealed unique properties, such as lasing, room temperature polariton condensation and the modification of excited electronic landscapes involved in molecular isomerization. Here we show that molecular vibrational modes of the electronic ground state can also be coherently coupled with a microcavity mode at room temperature, given the low vibrational thermal occupation factors associated with molecular vibrations, and the collective coupling of a large ensemble of molecules immersed within the cavity-mode volume. This enables the enhancement of the collective Rabi-exchange rate with respect to the single-oscillator coupling strength. The possibility of inducing large shifts in the vibrational frequency of selected molecular bonds should have immediate consequences for chemistry.

Suggested Citation

  • A. Shalabney & J. George & J. Hutchison & G. Pupillo & C. Genet & T. W. Ebbesen, 2015. "Coherent coupling of molecular resonators with a microcavity mode," Nature Communications, Nature, vol. 6(1), pages 1-6, May.
  • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms6981
    DOI: 10.1038/ncomms6981
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    Cited by:

    1. Rosario R. Riso & Tor S. Haugland & Enrico Ronca & Henrik Koch, 2022. "Molecular orbital theory in cavity QED environments," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    2. Connor K. Terry Weatherly & Justin Provazza & Emily A. Weiss & Roel Tempelaar, 2023. "Theory predicts UV/vis-to-IR photonic down conversion mediated by excited state vibrational polaritons," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. Irene Dolado & Carlos Maciel-Escudero & Elizaveta Nikulina & Evgenii Modin & Francesco Calavalle & Shu Chen & Andrei Bylinkin & Francisco Javier Alfaro-Mozaz & Jiahan Li & James H. Edgar & Fèlix Casan, 2022. "Remote near-field spectroscopy of vibrational strong coupling between organic molecules and phononic nanoresonators," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    4. Tao E. Li & Abraham Nitzan & Joseph E. Subotnik, 2022. "Energy-efficient pathway for selectively exciting solute molecules to high vibrational states via solvent vibration-polariton pumping," Nature Communications, Nature, vol. 13(1), pages 1-8, December.
    5. Kaihong Sun & Raphael F. Ribeiro, 2024. "Theoretical formulation of chemical equilibrium under vibrational strong coupling," Nature Communications, Nature, vol. 15(1), pages 1-12, December.
    6. Sindhana Pannir-Sivajothi & Jorge A. Campos-Gonzalez-Angulo & Luis A. Martínez-Martínez & Shubham Sinha & Joel Yuen-Zhou, 2022. "Driving chemical reactions with polariton condensates," Nature Communications, Nature, vol. 13(1), pages 1-9, December.
    7. Tingting Wu & Chongwu Wang & Guangwei Hu & Zhixun Wang & Jiaxin Zhao & Zhe Wang & Ksenia Chaykun & Lin Liu & Mengxiao Chen & Dong Li & Song Zhu & Qihua Xiong & Zexiang Shen & Huajian Gao & Francisco J, 2024. "Ultrastrong exciton-plasmon couplings in WS2 multilayers synthesized with a random multi-singular metasurface at room temperature," Nature Communications, Nature, vol. 15(1), pages 1-9, December.

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