Plasmon–Exciton Strong Coupling in Colloidal Au Nanocubes with Layered Molecular J-Aggregates

Strong coupling between light and matter forms hybrid states, such as exciton–polaritons, which are crucial for advancements in quantum science and technology. Plasmonic metal nanoparticles, with their ultrasmall mode volumes, are effective for generating these states, but the coupling strength is often limited by surface saturation of excitonic materials. Additionally, cubic nanoparticles, which can generate strong local fields, have not been systematically explored. This study investigates strong coupling in Au nanocubes (AuNCs) coupled with J-aggregates, observing spectral splitting in both extinction and scattering spectra. Our findings suggest that smaller AuNCs, with higher-quality resonances and reduced mode volumes, achieve stronger coupling. Furthermore, a layer-by-layer (LBL) coating of J-aggregates on AuNCs results in a ∼21% increase in coupling strength. Simulations reveal the mechanism behind the enhanced coupling and confirm that the layering method effectively increases coupling, surpassing the limitations of the finite surface area of nanoparticles.