MAURO, L; CAICEDO, K; JONUSAUSKAS, G; AVRILLER, Rémi

doi:10.1103/PhysRevB.103.165412

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Physical Review B: Condensed Matter and Materials Physics (1998-2015). 2021-04-13

American Physical Society

Résumé en anglais

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.< Réduire

Mots clés en anglais

Atoms

ions

molecules in cavities

Chemical physics and physical chemistry

Polaritons

Light-latter interaction

Optical microcavities

DOI

http://dx.doi.org/10.1103/PhysRevB.103.165412

Project ANR

Réactions Chimiques, Transfert de Charges et d'Energie en Cavité Electromagnétique - ANR-18-CE30-0006
University of Bordeaux Graduate Scholl in Light Sciences & Technologies - ANR-17-EURE-0027

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Laboratoire Ondes et Matière d'Aquitaine (LOMA) - UMR 5798