A quantum optics approach to photoinduced electron transfer in cavities.


Journal

The Journal of chemical physics
ISSN: 1089-7690
Titre abrégé: J Chem Phys
Pays: United States
ID NLM: 0375360

Informations de publication

Date de publication:
07 Feb 2021
Historique:
entrez: 9 2 2021
pubmed: 10 2 2021
medline: 10 2 2021
Statut: ppublish

Résumé

We study a simple model for photoinduced electron transfer reactions for the case of many donor-acceptor pairs that are collectively and homogeneously coupled to a photon mode of a cavity. We describe both coherent and dissipative collective effects resulting from this coupling within the framework of a quantum optics Lindblad master equation. We introduce a method to derive an effective rate equation for electron transfer by adiabatically eliminating donor and acceptor states and the cavity mode. The resulting rate equation is valid for both weak and strong coupling to the cavity mode and describes electronic transfer through both the cavity-coupled bright states and the uncoupled dark states. We derive an analytic expression for the instantaneous electron transfer rate that depends non-trivially on the time-varying number of pairs in the ground state. We find that under proper resonance conditions, and in the presence of an incoherent drive, reaction rates can be enhanced by the cavity. This enhancement persists, and can even be largest, in the weak light-matter coupling regime. We discuss how the cavity effect is relevant for realistic experiments.

Identifiants

pubmed: 33557545
doi: 10.1063/5.0037412
doi:

Types de publication

Journal Article

Langues

eng

Sous-ensembles de citation

IM

Pagination

054104

Auteurs

D Wellnitz (D)

ISIS (UMR 7006), University of Strasbourg and CNRS, and icFRC, 67000 Strasbourg, France.

G Pupillo (G)

ISIS (UMR 7006), University of Strasbourg and CNRS, and icFRC, 67000 Strasbourg, France.

J Schachenmayer (J)

ISIS (UMR 7006), University of Strasbourg and CNRS, and icFRC, 67000 Strasbourg, France.

Classifications MeSH