Sculpting ultrastrong light-matter coupling through spatial matter structuring.

The central theme of cavity quantum electrodynamics is the coupling of a single optical mode with a single matter excitation, leading to a doublet of cavity polaritons which govern the optical properties of the coupled structure. Especially in the ultrastrong coupling regime, where the ratio of the vacuum Rabi frequency and the quasi-resonant carrier frequency of light, Ω/ , approaches unity, the polariton doublet bridges a large spectral bandwidth 2Ω, and further interactions with off-resonant light and matter modes may occur. The resulting multi-mode coupling has recently attracted attention owing to the additional degrees of freedom for designing light-matter coupled resonances, despite added complexity.

Mode-multiplexing deep-strong light-matter coupling.

Dressing electronic quantum states with virtual photons creates exotic effects ranging from vacuum-field modified transport to polaritonic chemistry, and squeezing or entanglement of modes. The established paradigm of cavity quantum electrodynamics maximizes the light-matter coupling strength , defined as the ratio of the vacuum Rabi frequency and the frequency of light, by resonant interactions. Yet, the finite oscillator strength of a single electronic excitation sets a natural limit to .

Non-adiabatic stripping of a cavity field from deep-strongly coupled electrons.

Atomically strong light pulses can drive sub-optical-cycle dynamics. When the Rabi frequency - the rate of energy exchange between light and matter - exceeds the optical carrier frequency, fascinating non-perturbative strong-field phenomena emerge, such as high-harmonic generation and lightwave transport. Here, we explore a related novel subcycle regime of ultimately strong light-matter interaction without a coherent driving field.

Tailored Subcycle Nonlinearities of Ultrastrong Light-Matter Coupling.

We explore the nonlinear response of tailor-cut light-matter hybrid states in a novel regime, where both the Rabi frequency induced by a coherent driving field and the vacuum Rabi frequency set by a cavity field are comparable to the carrier frequency of light. In this previously unexplored strong-field limit of ultrastrong coupling, subcycle pump-probe and multiwave mixing nonlinearities between different polariton states violate the normal-mode approximation while ultrastrong coupling remains intact, as confirmed by our mean-field model. We expect such custom-cut nonlinearities of hybridized elementary excitations to facilitate nonclassical light sources, quantum phase transitions, or cavity chemistry with virtual photons.