Ultrastrong coupling of polar phonons and effective epsilon-near-zero modes in coaxial nanocavities

Abstract

Ultrastrong coupling (USC), where the light-matter coupling strength is comparable to the resonance frequency of the uncoupled bare system, presents new frontiers in nanophotonics. However, it has remained notoriously difficult to achieve experimentally. Here we demonstrate USC between polar phonons and mid-infrared (MIR) light in coaxial nanocavities. We achieved a level splitting of strongly coupled polaritons of 50% of the resonant frequency, enabled by the effective epsilon-near-zero (ENZ) responses in the MIR of the SiO2-filled coaxial nanocavities. We theoretically describe this unusually large level splitting as USC using a 2x2 matrix form derived from the coupling of polar phonon lattice and Maxwell's equations. Our wafer-scale coaxial ENZ nanocavity platform offers new routes to explore the physics of vibrational USC within polaritonic systems and harness a broad range of resonant transitions in the MIR regime.