Ultrastrong Light-Matter Coupling in Materials

Abstract: Ultrastrong light-matter coupling has traditionally been studied in optical cavities, where it occurs when the light-matter coupling strength reaches a significant fraction of the transition frequency. This regime fundamentally alters the ground and excited states of the particle-cavity system, unlocking new ways to control its physics and chemistry. However, achieving ultrastrong coupling in engineered cavities remains a major challenge. Here, we show that ultra- and deep-strong coupling naturally occur in bulk materials without the need for external cavities. By analyzing experimental data from over 70 materials, we demonstrate that phonon-, exciton-, and plasmon-polaritons in many solids exhibit ultrastrong coupling, systematically surpassing the coupling strengths achieved in cavity-based systems. To explain this phenomenon, we introduce a dipole lattice model based on a generalized Hopfield Hamiltonian, which unifies photon-matter, matter-matter, and photon-photon interactions. The complete overlap between the photonic and collective dipole modes in the lattice enables ultrastrong coupling, leading to excited-state mixing, radiative decay suppression, and potential phase transitions into collective ground states. Applying our model to real materials, we show that it reproduces light-matter coupling across broad material classes and may underlie structural phase transitions that give rise to emergent phenomena such as ferroelectricity, insulator-to-metal transitions, and exciton condensation. Recognizing ultrastrong coupling as an intrinsic property of solids reshapes our understanding of light-matter interactions and opens new avenues for exploring quantum materials and exotic phases of matter.