Abstract:This Letter describes strong coupling between a plasmonic nanoparticle (NP) lattice cavity and Soret excitons in a metal−organic framework (MOF) film. In optical transmission measurements, we observed a lower polariton mode that can be spectrally tuned by infiltrating MOF pores with solvents of different refractive index. Using transient absorption spectroscopy, both the lower and upper polariton modes can be resolved, with an estimated Rabi splitting of ∼300 meV, nearly twice that of other plasmonic cavity−or… Show more
“…Plasmonic nanoparticle lattices are advantageous cavities for strong coupling and for carrying out chemical reactions due to their open lattice structure. [34][35][36][37] Periodic lattices of metallic nanoparticles can support high-quality surface lattice resonance (SLR) cavity modes by coupling the localized surface plasmons of each nanoparticle to the diffractive photonic modes in the lattice in an index-matched environment. [38][39] The single substrate and metal nanoparticles of the cavity facilitate incorporation into spectroelectrochemistry experiments, as the cavity is accessible to solvents and reagents, and the lattices can be fabricated on transparent conductive substrates.…”
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.
“…Plasmonic nanoparticle lattices are advantageous cavities for strong coupling and for carrying out chemical reactions due to their open lattice structure. [34][35][36][37] Periodic lattices of metallic nanoparticles can support high-quality surface lattice resonance (SLR) cavity modes by coupling the localized surface plasmons of each nanoparticle to the diffractive photonic modes in the lattice in an index-matched environment. [38][39] The single substrate and metal nanoparticles of the cavity facilitate incorporation into spectroelectrochemistry experiments, as the cavity is accessible to solvents and reagents, and the lattices can be fabricated on transparent conductive substrates.…”
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.
“…Plasmonic nanoparticle lattices are advantageous cavities for strong coupling and for carrying out chemical reactions due to their open lattice structure. − Periodic lattices of metallic nanoparticles can support high-quality surface lattice resonance (SLR) cavity modes by coupling the localized surface plasmons of each nanoparticle to the diffractive photonic modes in the lattice in an index-matched environment. , The single substrate and metal nanoparticles of the cavity facilitate incorporation into spectroelectrochemistry experiments, as the cavity is accessible to solvents and reagents, and the lattices can be fabricated on transparent conductive substrates . By tuning nanoparticle material and shape as well as periodicity, plasmonic lattice cavities can be designed to interact with different excitonic materials …”
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 are 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.
Strong coupling between surface plasmon resonance (SPR) modes and excitons holds great potential for many chemical and physical applications. However, a clear understanding on how far‐field spectral characteristics of SPR (linewidths and intensity) affect the coupling strength remains unclear because these parameters are difficult to be individually tuned. These spectral characteristics are associated with the damping rate and field enhancement that depend on the morphology of the plasmonic nanostructure. In this work, the influence of the SPR line shape on exciton‐plasmon coupling is systematically investigated by delicately tuning the linewidths and resonance intensities of the plasmonic arrays. It is found that the SPR modes with narrow linewidths or large intensity are favorable for the exciton–plasmon system to achieve strong coupling. The obtained clear relationships between the SPR line shape and coupling strength provide guidance for the design and optimization of exciton‐plasmon coupling systems, favoring the highly efficient manipulation of exciton polaritons and enabling specific applications driven by strong coupling.
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