Electrochemical Control of Strong Coupling of CdSe Exciton-Polaritons in Plasmonic Cavities

16 April 2024, Version 1
This content is a preprint and has not undergone peer review at the time of posting.

Abstract

This work reports in-situ (active) electrochemical control over the coupling strength between semiconducting nanoplatelets and a plasmonic cavity. We found that by applying a reductive bias to an Al nanoparticle lattice working electrode, the number of CdSe nanoplatelet emitters that can couple to the cavity is decreased. Strong coupling can be reversibly recovered by discharging the lattice at oxidative potentials relative to the conduction band edge reduction potential of the emitters. By correlating the number of electrons added or removed with the measured coupling strength, we identified that loss and recovery of strong coupling is likely hindered by side processes that trap and/or inhibit electrons from populating the nanoplatelet conduction band. These findings demonstrate tunable, external control of strong coupling and offer prospects to tune selectivity in chemical reactions.

Supplementary materials

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Supporting Information
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Lattice and NPL film substrate fabrication, experimental conditions of spectroelectrochemical experiments performed, sigmoidal fit equation parameters for quantification of nanoplatelet conduction band edge potential, FDTD modeling of uncoupled cavity, fitting procedures, spectroelectrochemical linear sweep voltammetry of coupled film and cavity, chronoamperometry of angle-dependent transmission spectroelectrochemical measurements, fitting with the coupled oscillator model and quantification of gHH as a function of cycled potential (PDF)
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