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

Tao E. Li (), Abraham Nitzan () and Joseph E. Subotnik ()
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Tao E. Li: University of Pennsylvania
Abraham Nitzan: University of Pennsylvania
Joseph E. Subotnik: University of Pennsylvania

Nature Communications, 2022, vol. 13, issue 1, 1-8

Abstract: 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 (

Date: 2022
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DOI: 10.1038/s41467-022-31703-8

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