Many-molecule reaction triggered by a single photon in polaritonic chemistry

Abstract

The second law of photochemistry states that in most cases, no more than one molecule is activated for an excited-state reaction for each photon absorbed by a collection of molecules. In this work, we demonstrate that it is possible to trigger a many-molecule reaction using only one photon by strongly coupling the molecular ensemble to a confined light mode. The collective nature of the resulting hybrid states of the system (the so-called polaritons) leads to the formation of a polaritonic "supermolecule" involving the degrees of freedom of all molecules, opening a reaction path on which all involved molecules undergo a chemical transformation. We theoretically investigate the system conditions for this effect to take place and be enhanced.

arXiv comment5 pages, 2 figures

References in corpus (9)

• Interfacing single photons and single quantum dots with photonic nanostructures
• Cavity-controlled chemistry in molecular ensembles
• Atoms and Molecules in Cavities: From Weak to Strong Coupling in QED Chemistry
• Realizing strong light-matter interactions between single nanoparticle plasmons and molecular excitons at ambient conditions
• Cavity-induced modifications of molecular structure in the strong coupling regime
• Suppressing photochemical reactions with quantized light fields
• Plasmon-Exciton-Polariton Lasing
• Cavity Born-Oppenheimer Approximation for Correlated Electron-Nuclear-Photon Systems
• Non-adiabatic dynamics of molecules in optical cavities

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