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Energy-efficient pathway for selectively exciting solute molecules to high vibrational states via solvent vibration-polariton pumping

Author

Listed:
  • Tao E. Li

    (University of Pennsylvania
    Yale University)

  • Abraham Nitzan

    (University of Pennsylvania
    Tel Aviv University)

  • Joseph E. Subotnik

    (University of Pennsylvania)

Abstract

Selectively exciting target molecules to high vibrational states is inefficient in the liquid phase, which restricts the use of IR pumping to catalyze ground-state chemical reactions. Here, we demonstrate that this inefficiency can sometimes be solved by confining the liquid to an optical cavity under vibrational strong coupling conditions. For a liquid solution of 13CO2 solute in a 12CO2 solvent, cavity molecular dynamics simulations show that exciting a polariton (hybrid light-matter state) of the solvent with an intense laser pulse, under suitable resonant conditions, may lead to a very strong (>3 quanta) and ultrafast (

Suggested Citation

  • 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.
    • Handle: RePEc:nat:natcom:v:13:y:2022:i:1:d:10.1038_s41467-022-31703-8
    DOI: 10.1038/s41467-022-31703-8
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    References listed on IDEAS

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    1. 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.
    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.
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    Cited by:

    1. 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.
    2. 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.

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