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Excited-state vibration-polariton transitions and dynamics in nitroprusside

Author

Listed:
  • Andrea B. Grafton

    (National Research Council Post-Doctoral Scholar)

  • Adam D. Dunkelberger

    (Naval Research Laboratory)

  • Blake S. Simpkins

    (Naval Research Laboratory)

  • Johan F. Triana

    (Universidad de Santiago de Chile)

  • Federico J. Hernández

    (Queen Mary University of London)

  • Felipe Herrera

    (Universidad de Santiago de Chile)

  • Jeffrey C. Owrutsky

    (Naval Research Laboratory)

Abstract

Strong cavity coupling to molecular vibrations creates vibration-polaritons capable of modifying chemical reaction kinetics, product branching ratios, and charge transfer equilibria. However, the mechanisms impacting these molecular processes remain elusive. Furthermore, even basic elements determining the spectral properties of polaritons, such as selection rules, transition moments, and lifetimes are poorly understood. Here, we use two-dimensional infrared and filtered pump–probe spectroscopy to report clear spectroscopic signatures and relaxation dynamics of excited vibration-polaritons formed from the cavity-coupled NO band of nitroprusside. We apply an extended multi-level quantum Rabi model that predicts transition frequencies and strengths that agree well with our experiment. Notably, the polariton features decay ~3–4 times slower than the polariton dephasing time, indicating that they support incoherent population, a consequence of their partial matter character.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-020-20535-z
    DOI: 10.1038/s41467-020-20535-z
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    Cited by:

    1. 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.
    2. Qi Yu & Joel M. Bowman, 2023. "Manipulating hydrogen bond dissociation rates and mechanisms in water dimer through vibrational strong coupling," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    3. 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.
    4. Fan Wu & Daniel Finkelstein-Shapiro & Mao Wang & Ilmari Rosenkampff & Arkady Yartsev & Torbjörn Pascher & Tu C. Nguyen- Phan & Richard Cogdell & Karl Börjesson & Tönu Pullerits, 2022. "Optical cavity-mediated exciton dynamics in photosynthetic light harvesting 2 complexes," Nature Communications, Nature, vol. 13(1), pages 1-7, December.

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