In quantum electrodynamics, the choice of gauge influences the form of light–matter interactions. However, gauge invariance implies that all physical results should be independent of this formal choice. The Rabi model, a widespread description for the dipolar coupling between a two-level atom and a quantized electromagnetic field, seemingly violates this principle in the presence of ultrastrong light–matter coupling, a regime that is now experimentally accessible in many physical systems. This failure is attributed to the finite-level truncation of the matter system, an approximation that enters the derivation of the Rabi model. Here, we identify the source of gauge violation and provide a general method for the derivation of light–matter Hamiltonians in truncated Hilbert spaces that produces gauge-invariant physical results, even for extreme light–matter interaction regimes. This is achieved by compensating the non-localities introduced in the construction of the effective Hamiltonians. The resulting quantum Rabi Hamiltonian in the Coulomb gauge differs significantly in form from the standard one, but provides the same physical results obtained by using the dipole gauge. These results shed light on gauge invariance in the non-perturbative and extreme-interaction regimes, and solve long-lasting controversies arising from gauge ambiguities in the quantum Rabi and Dicke models.

Ultrastrong coupling between light and matter has, in the past decade, transitioned from a theoretical idea to an experimental reality. It is a new regime of quantum light–matter interaction, which goes beyond weak and strong coupling to make the coupling strength comparable to the transition frequencies in the system. The achievement of weak and strong coupling has led to increased control of quantum systems and to applications such as lasers, quantum sensing, and quantum information processing. Here we review the theory of quantum systems with ultrastrong coupling, discussing entangled ground states with virtual excitations, new avenues for nonlinear optics, and connections to several important physical models. We also overview the multitude of experimental setups, including superconducting circuits, organic molecules, semiconductor polaritons, and optomechanical systems, that have now achieved ultrastrong coupling. We conclude by discussing the many potential applications that these achievements enable in physics and chemistry.

We consider two separate atoms interacting with a single-mode optical or microwave resonator. When the frequency of the resonator field is twice the atomic transition frequency, we show that there exists a resonant coupling between one photon and two atoms, via intermediate virtual states connected by counterrotating processes. If the resonator is prepared in its one-photon state, the photon can be jointly absorbed by the two atoms in their ground state which will both reach their excited state with a probability close to one. Like ordinary quantum Rabi oscillations, this process is coherent and reversible, so that two atoms in their excited state will undergo a downward transition jointly emitting a single cavity photon. This joint absorption and emission process can also occur with three atoms. The parameters used to investigate this process correspond to experimentally demonstrated values in circuit quantum electrodynamics systems.