Paramagnets as a platform for Dicke physics

The interaction of an ensemble of two-level atoms and a quantized electromagnetic field, described by the Dicke Hamiltonian, is an extensively studied problem in quantum optics. However, experimental efforts to explore similar physics in condensed matter typically employ bosonic matter modes (e.g., phonons, magnons, and plasmons) that are describable as simple harmonic oscillators, i.e., an infinite ladder of equally spaced energy levels. Here, we examine ultrastrong coupling between a coherent light mode and an ensemble of paramagnetic spins, a finite-multilevel system, in Gd₃Ga₅O₁₂. The electron paramagnetic resonance of Gd³⁺ ions is tuned by a magnetic field into resonance with a Fabry-Pérot cavity mode, resulting in the formation of spin-photon hybrid states, or Zeeman polaritons. We observe that the light-matter coupling strength, measured through the vacuum Rabi splitting, decreases with increasing temperature, which can be explained by the temperature-dependent population difference between the lower and higher-energy states, a trait of a finite-level system. This finding demonstrates that a spin-boson system is more compatible with the Dicke model and has advantages over boson-boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light-matter hybrids.