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

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 (<1 ps) excitation of the solute, even though the solvent ends up being barely excited. By contrast, outside a cavity the same

SUBMITTER: Li TE 

PROVIDER: S-EPMC9300737 | biostudies-literature | 2022 Jul

REPOSITORIES: biostudies-literature