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.
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.
We investigate the nonlinearities of custom-tailored ultrastrongly light-matter coupled states by driving them with both the vacuum electromagnetic field and strong coherent THz waveforms. In this novel regime, where both the Rabi frequency induced by the coherent field and the vacuum Rabi frequency set by the cavity field are on the order of the carrier frequency of light, we observe strong subcycle pump-probe and multiwave mixing nonlinearities and nonlinear polariton correlations, violating the normal-mode approximation. Such custom-cut nonlinearities of hybridized excitations set the stage for nonlinear optical control of deep-strong coupling, exploring quantum phase transitions or nonclassical light sources.
Dressing quantum states of matter with virtual photons can create exotic effects ranging from vacuum-field modified transport to polaritonic chemistry, and may drive strong squeezing or entanglement of light and matter modes. The established paradigm of cavity quantum electrodynamics focuses on resonant light-matter interaction to maximize the coupling strength ΩR/ωc, defined as the ratio of the vacuum Rabi frequency and the carrier frequency of light. Yet, the finite oscillator strength of a single electronic excitation sets a natural limit to ΩR/ωc. Here, we demonstrate a new regime of record-strong light-matter interaction which exploits the cooperative dipole moments of multiple, highly non-resonant magnetoplasmon modes specifically tailored by our metasurface. This multi-mode coupling creates an ultrabroadband spectrum of over 20 polaritons spanning 6 optical octaves, vacuum ground state populations exceeding 1 virtual excitation quantum for electronic and optical modes, and record coupling strengths equivalent to ΩR/ωc=3.19. The extreme interaction drives strongly subcycle exchange of vacuum energy between multiple bosonic modes akin to high-order nonlinearities otherwise reserved to strong-field physics, and entangles previously orthogonal electronic excitations solely via vacuum fluctuations of the common cavity mode. This offers avenues towards tailoring phase transitions by coupling otherwise non-interacting modes, merely by shaping the dielectric environment.
Dressing electrons with the vacuum electromagnetic field of an optical microresonator can lead to the creation of new states of matter. When the rate of energy exchange between the two systems, the vacuum Rabi frequency, Ω R , becomes comparable to the carrier frequency of light, ω 0 , the regime of ultrastrong coupling is reached [1] . Here, anti-resonant interactions result in a modified vacuum ground state and give rise to novel phenomena of cavity quantum electrodynamics (c-QED), such as the vacuum Bloch-Siegert shift [2] . When Ω R even surpasses ω 0 , deepstrong coupling is attained [3] , [4] . While the exploration of the equilibrium properties of this extreme setting has just begun, its subcycle dynamics is expected to reveal qualitatively new quantum phenomena.
We consider a generalized version of the Rabi model that includes a nonlinear, dispersive-type atom-field interaction in addition to the usual linear dipole coupling, as well as cavity dissipation. An effective system of this sort arises, for example, in a quantum simulation of the Rabi model based upon Raman transitions in an optical cavity QED setting [A. L. Grimsmo and S. Parkins, Phys. Rev. A 87, 033814 (2013)]. For a range of the nonlinear interaction strength about a special value, degeneracies or near degeneracies of the states in the cavity-mode vacuum and single-photon subspaces, in combination with cavity loss, gives rise to an essentially closed cycle of excitations and photon emissions within these subspaces. Consequently, the cavity output field is strongly antibunched, while over this range of nonlinear strengths the atomic population undergoes an abrupt inversion. We develop a quantum-trajectory-based description of the system that models its key properties very well, and use a simple dressed-state picture to explain the novel structure of the cavity fluorescence spectrum. We also present numerical results for a potential realization of the system using a rubidium atom coupled strongly to a high-finesse optical cavity mode.
Interaction of the vacuum field of an optical mode with an electronic two-level system can drive non-perturbative light-matter dynamics, resulting in an exotic quantum ground state containing a sizeable population of virtual excitations. In the deep-strong coupling (DSC) regime, where the Rabi frequency,ΩR, exceeds the eigen-frequencies of the coupled systems, this extreme ground state can result in spectacular effects of cavity-QED, such as the expected release of the virtual photon ground state population as vacuum radiation by non-adiabatic modulation of the coupling mechanism [1], [2]. However, for resonant coupling of two single modes [3], the finite oscillator strength of resonant electronic excitation sets a natural limit to the achievable coupling strength, hindering further exploration of this exciting field.
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.