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Charge-Transfer Chemical Reactions in Nanofluidic Fabry-Pérot Cavities

Abstract : We investigate the chemical reactivity of molecular populations confined inside a nanofluidic Fabry-Pérot cavity. Due to strong light-matter interactions developing between a resonant electromagnetic cavity-mode and the electric dipole moment of the confined molecules, a polariton is formed. The former gets dressed by environmental vibrational and rotational degrees of freedom of the solvent. We call the resulting polariton dressed by its cloud of environmental excitation a "reacton", since it further undergoes chemical reactions. We characterize how the reacton formation modifies the kinetics of a photoisomerization chemical reaction involving an elementary charge-transfer process. We show that the reaction driving-force and reorganization energy are both modulated optically by the reactant concentration, the vacuum Rabi splitting and the de-tuning between the Fabry-Pérot cavity frequency and targeted electronic transition. Finally, we compute the ultrafast picosecond dynamics of the whole photochemical reaction. We predict that despite optical cavity losses and solvent-mediated non-radiative relaxation, measurable signatures of the reacton formation can be found in state-of-the-art pump-probe experiments.
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https://hal.archives-ouvertes.fr/hal-02962814
Contributor : Rémi Avriller <>
Submitted on : Friday, October 9, 2020 - 3:01:08 PM
Last modification on : Monday, April 19, 2021 - 1:44:30 PM
Long-term archiving on: : Sunday, January 10, 2021 - 6:45:54 PM

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L Mauro, K Caicedo, G Jonusauskas, Rémi Avriller. Charge-Transfer Chemical Reactions in Nanofluidic Fabry-Pérot Cavities. Physical Review B: Condensed Matter and Materials Physics (1998-2015), American Physical Society, 2021, ⟨10.1103/PhysRevB.103.165412⟩. ⟨hal-02962814⟩

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