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Conference on Lasers and Electro-Optics Europe & European Quantum Electronics Conference (CLEO/Europe-EQEC)

Multi-Octave Deep-Strong Light-Matter Coupling of Multiple Modes

Joshua Mornhinweg, Laura K. Diebel, Maike Halbhuber, Viola Zeller, Josef Riepl, Tobias Inzenhofer, Dominique Bougeard, R. Huber, C. Lange

Published Jun 26, 2023• 0 citations
Publisher

Abstract

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,$\Omega_{\mathrm{R}}$, 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.

DOI
10.1109/cleo/europe-eqec57999.2023.10231621

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•Jan 1, 2018•28 citations
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\Omega_{\mathrm{R}}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.
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/ωcΩ_\mathrm{R}/ω_\mathrm{c}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/ωcΩ_\mathrm{R}/ω_\mathrm{c}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=3.19Ω_\mathrm{R}/ω_\mathrm{c}=3.19ΩR​/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.
The prototypical system constituted by a two-level atom interacting with a quantized single-mode electromagnetic field is described by the quantum Rabi model (QRM). The QRM is potentially valid at any light-matter interaction regime, ranging from the weak (where the decay rates exceeds the coupling rate) to the deep strong coupling (where the interaction rate exceeds the bare transition frequencies of the subsystems). However, when reaching the ultrastrong coupling regime, several theoretical issues may prevent the correct description of the observable dynamics of such a system: (i) the standard quantum optics master equation fails to correctly describe the interaction of this system with the reservoirs; (ii) the correct output photon rate is no longer proportional to the intracavity photon number; and (iii) they appear to violate gauge invariance. Here, we study the photon flux emission rate of this system under the incoherent excitation of the two-level atom for any light-matter interaction strength and consider different effective temperatures. The dependence of the emission spectra on the coupling strength is the result of the interplay between energy levels, matrix elements of the observables, and the density of states of the reservoirs. Within this approach, we also study the occurrence of light-matter decoupling in the deep strong-coupling regime and show how all of the obtained results are gauge invariant.
Recent technological developments have made it increasingly easy to access the non-perturbative regimes of cavity quantum electrodynamics known as ultrastrong or deep strong coupling, where the light-matter coupling becomes comparable to the bare modal frequencies. In this work, we address the adequacy of the broadly used single-mode cavity approximation to describe such regimes. We demonstrate that, in the non-perturbative light-matter coupling regimes, the single-mode models become unphysical, allowing for superluminal signalling. Moreover, considering the specific example of the quantum Rabi model, we show that the multi-mode description of the electromagnetic field, necessary to account for light propagation at finite speed, yields physical observables that differ radically from their single-mode counterparts already for moderate values of the coupling. Our multi-mode analysis also reveals phenomena of fundamental interest on the dynamics of the intracavity electric field, where a free photonic wavefront and a bound state of virtual photons are shown to coexist.
Traditionally, strong-field physics explores phenomena in laser-driven matter (atoms, molecules, and solids) that cannot be understood by treating the laser field as a small perturbation. Therefore, the presence of an extremely strong external field is usually a prerequisite for observing strong-field phenomena. However, even in the complete absence of an external electromagnetic field, strong-field phenomena can arise when matter strongly couples with the zero-point field of the quantum vacuum state, i.e., fluctuating electromagnetic waves whose expectation value is zero. This can occur in free space where the matter strongly interacts with a continuum of photon modes, but some of the most striking examples of strong-field physics without an external field occur in a cavity setting, in which an ensemble of two-level atoms resonantly interacts with a single photonic mode of vacuum fields, producing vacuum Rabi splitting. In particular, the nature of the matter-vacuum-field coupled system fundamentally changes when the coupling rate (equal to one half of the vacuum Rabi splitting) becomes comparable to, or larger than, the resonance frequency. In this so-called ultrastrong coupling regime, a non-negligible number of photons exist in the ground state of the coupled system. Furthermore, the coupling rate can be cooperatively enhanced (via so-called Dicke cooperativity) when the matter is comprised of a large number of identical two-level particles, and a quantum phase transition is predicted to occur as the coupling rate reaches a critical value. Low-energy electronic or magnetic transitions in many-body condensed matter systems with large dipole moments are ideally suited for searching for these predicted phenomena. Here, we discuss two condensed matter systems that have shown cooperative ultrastrong interactions in the terahertz frequency range: a Landau-quantized two-dimensional electron gas interacting with high-quality-factor cavity photons, and an Er3+ spin ensemble interacting with Fe3+ magnons in ErFeO3.
Abstract Recent technological developments have made it increasingly easy to access the non-perturbative regimes of cavity quantum electrodynamics known as ultrastrong or deep strong coupling, where the light–matter coupling becomes comparable to the bare modal frequencies. In this work, we address the adequacy of the broadly used single-mode cavity approximation to describe such regimes. We demonstrate that, in the non-perturbative light–matter coupling regimes, the single-mode models become unphysical, allowing for superluminal signalling. Moreover, considering the specific example of the quantum Rabi model, we show that the multi-mode description of the electromagnetic field, necessary to account for light propagation at finite speed, yields physical observables that differ radically from their single-mode counterparts already for moderate values of the coupling. Our multi-mode analysis also reveals phenomena of fundamental interest on the dynamics of the intracavity electric field, where a free photonic wavefront and a bound state of virtual photons are shown to coexist.