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Light-matter strong coupling is defined when the coupling strength exceeds the losses in the system, whereas ultrastrong coupling is not simply strong coupling with even larger coupling strength. Instead, ultrastrong coupling regime arises when the coupling strength is comparable to the transition frequency in the system. At present, ultrastrong light-matter interactions have been achieved in superconducting circuits, semiconductor polaritons, and organic molecules, where these systems are typically at the micrometer scale. In this work, we investigated ultrastrong coupling in a nanoparticle plexcitonic system, i.e. a single gold nanocube coated with quantum emitters and positioned on a gold film. We observed a normalized coupling rate  η  ~ 0.12 to the antenna mode in such coated nanocube-on-mirror ( c -NCoM) configuration at the multilayer emitter level. In contrast to the gap mode that squeezes all the optical fields into the gap region, the antenna mode in  c -NCoM provides multiple exterior hot spots at the upper corners of the nanocube, which can be exploited for qubit entanglement within a single nanocube. The concurrence between adjacent emitters is estimated up to 0.6. This theoretical study establishes a promising route toward building a scalable quantum network using single plexcitonic nanocubes as quantum nodes.

Ultrastrong coupling in single plexcitonic nanocubes