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The realization of higher coupling strengths between coupled resonant modes enables exploration of compelling phenomena in diverse fields of physics and chemistry. In this study, we focus on the modal coupling between localized surface plasmon resonance (LSPR) of Au nanoparticles (Au-NPs) and Fabry–Pérot mode (p-NiO/Au film). The effects of nanoparticle size, projected surface coverage (PSC), interparticle distance (IPD), and arrangement to the coupling strength between the two modes are theoretically investigated using finite-difference time-domain (FDTD) method. Au-NPs/p-NiO/Au film (ANA) nanostructures with NPs size of 10 nm, 30 nm, and 50 nm are considered. Numerical calculations point to larger size and higher projected surface coverage (also smaller IPD) of NPs as pre-eminent factors in enhancing the strength of modal coupling. ANA nanostructure with NPs size of 30 nm (ANA-30) and 50 nm (ANA-50) are experimentally fabricated via a facile air–liquid interface self-assembly. The fabricated nanodevices exhibit immense Rabi splitting energies of 655 meV (ANA-30) and 770 meV (ANA-50), and thus fulfill the ultrastrong coupling condition with remarkable splitting energy to bare (plasmon) energy ratio of 0.35 (ANA-30) and 0.4 (ANA-50). The physical insights presented in this study, together with the simple and scalable fabrication process, establish a viable approach to realize stronger coupling between LSPR and Fabry–Pérot mode in metal NPs/dielectric/metal film systems. This will be vital to take advantage of the promising performance enhancements of plasmonic-based nanostructures under strongly coupled regimes in areas such as solar to fuel conversion, sensing, opto-electronics, and quantum applications.

Realization of ultrastrong coupling between LSPR and Fabry–Pérot mode via self-assembly of Au-NPs on p-NiO/Au film