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Theory predicts UV/vis-to-IR photonic down conversion mediated by excited state vibrational polaritons

Author

Listed:
  • Connor K. Terry Weatherly

    (Northwestern University)

  • Justin Provazza

    (Northwestern University)

  • Emily A. Weiss

    (Northwestern University)

  • Roel Tempelaar

    (Northwestern University)

Abstract

This work proposes a photophysical phenomenon whereby ultraviolet/visible (UV/vis) excitation of a molecule involving a Franck-Condon (FC) active vibration yields infrared (IR) emission by strong coupling to an optical cavity. The resulting UV/vis-to-IR photonic down conversion process is mediated by vibrational polaritons in the electronic excited state potential. It is shown that the formation of excited state vibrational polaritons (ESVP) via UV/vis excitation only involve vibrational modes with both a non-zero FC activity and IR activity in the excited state. Density functional theory calculations are used to identify 1-Pyreneacetic acid as a molecule with this property and the dynamics of ESVP are modeled. Overall, this work introduces an avenue of polariton chemistry where excited state dynamics are influenced by the formation of vibrational polaritons. Along with this, the UV/vis-to-IR photonic down conversion is potentially useful in both sensing excited state vibrations and quantum transduction schemes.

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-40400-z
    DOI: 10.1038/s41467-023-40400-z
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    References listed on IDEAS

    as
    1. 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.
    2. Xinyang Li & Arkajit Mandal & Pengfei Huo, 2021. "Cavity frequency-dependent theory for vibrational polariton chemistry," Nature Communications, Nature, vol. 12(1), pages 1-9, December.
    3. 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.
    4. Lachlan P. Lindoy & Arkajit Mandal & David R. Reichman, 2023. "Quantum dynamical effects of vibrational strong coupling in chemical reactivity," Nature Communications, Nature, vol. 14(1), pages 1-14, December.
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