Spatially Encoded Polaritonic Ultra-Strong Coupling in Gradient Metasurfaces with Epsilon-Near-Zero Modes

Ultra-strong coupling (USC) is a light-matter interaction regime characterized by coupling strengths that substantially exceed the threshold for strong coupling. It gives rise to novel physical phenomena, such as efficient single-photon coupling and quantum gates, with applications in quantum sensing, nonlinear optics, and low-threshold lasing. Although early demonstrations in plasmonic systems have been realized, achieving USC in dielectric nanophotonic platforms, which offer lower losses and high Q-factors, remains challenging due to typically low mode overlap between the photonic field and the material resonance. Here, we demonstrate ultra-strong coupling to an epsilon-near-zero (ENZ) mode in an ultra-thin SiO$_2$ layer. Our approach leverages a dielectric dual-gradient metasurface supporting quasi-bound-states-in-the-continuum (qBIC) consisting of two tapered bars in each unit cell that generate strong out-of-plane electric fields which overlap exceptionally well with those of the ENZ mode. Using dual gradients to encode both the spectral and coupling parameter space, we track the anticrossing behaviour of this coupled system with high experimental precision, revealing a mode splitting equivalent to 19% of the ENZ mode energy; a four-to-five-fold increase compared to previous approaches. Furthermore, varying the position of the SiO$_2$ layer allows for deliberate control of the mode overlap and the coupling between the qBIC and either the ENZ mode or the transverse optical (TO) phonon can be selectively tuned. This allows us to experimentally create an USC three-resonator system, opening new possibilities for compact and scalable polaritonic devices for sensing and nonlinear optics.