The interaction of an ensemble of two-level atoms and a quantized electromagnetic field, described by the Dicke Hamiltonian, is an extensively studied problem in quantum optics. However, experimental efforts to explore similar physics in condensed matter typically employ bosonic matter modes (e.g., phonons, magnons, and plasmons) that are describable as simple harmonic oscillators, i.e., an infinite ladder of equally spaced energy levels. Here, we examine ultrastrong coupling between a coherent light mode and an ensemble of paramagnetic spins, a finite-multilevel system, in Gd$_3$Ga$_5$O$_{12}$. The electron paramagnetic resonance of Gd$^{3+}$ ions is tuned by a magnetic field into resonance with a Fabry--Pérot cavity mode, resulting in the formation of spin--photon hybrid states, or Zeeman polaritons. We observe that the light--matter coupling strength, measured through the vacuum Rabi splitting, decreases with increasing temperature, which can be explained by the temperature-dependent population difference between the lower and higher-energy states, a trait of a finite-level system. This finding demonstrates that a spin--boson system is more compatible with the Dicke model and has advantages over boson--boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light--matter hybrids.
The interaction of an ensemble of two-level atoms and a quantized electromagnetic field, described by the Dicke Hamiltonian, is an extensively studied problem in quantum optics. However, experimental efforts to explore similar physics in condensed matter typically employ bosonic matter modes (e.g., phonons, magnons, and plasmons) that are describable as simple harmonic oscillators, i.e., an infinite ladder of equally spaced energy levels. Here, we examine ultrastrong coupling between a coherent light mode and an ensemble of paramagnetic spins, a finite-multilevel system, in Gd3Ga5O12. The electron paramagnetic resonance of Gd3+ ions is tuned by a magnetic field into resonance with a Fabry--Pérot cavity mode, resulting in the formation of spin--photon hybrid states, or Zeeman polaritons. We observe that the light--matter coupling strength, measured through the vacuum Rabi splitting, decreases with increasing temperature, which can be explained by the temperature-dependent population difference between the lower and higher-energy states, a trait of a finite-level system. This finding demonstrates that a spin--boson system is more compatible with the Dicke model and has advantages over boson--boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light--matter hybrids.
The interaction of an ensemble of two-level atoms and a quantized electromagnetic field, described by the Dicke Hamiltonian, is an extensively studied problem in quantum optics. However, experimental efforts to explore similar physics in condensed matter typically employ bosonic matter modes (e.g., phonons, magnons, and plasmons) that are describable as simple harmonic oscillators, i.e., an infinite ladder of equally spaced energy levels. Here, we examine ultrastrong coupling between a coherent light mode and an ensemble of paramagnetic spins, a finite-multilevel system, in Gd3Ga5O12. The electron paramagnetic resonance of Gd3+ ions is tuned by a magnetic field into resonance with a Fabry–Pérot cavity mode, resulting in the formation of spin–photon hybrid states, or Zeeman polaritons. We observe that the light–matter coupling strength, measured through the vacuum Rabi splitting, decreases with increasing temperature, which can be explained by the temperature-dependent population difference between the lower and higher-energy states, a trait of a finite-level system. This finding demonstrates that a spin–boson system is more compatible with the Dicke model and has advantages over boson–boson systems for pursuing experimental realizations of phenomena predicted for ultrastrongly coupled light–matter hybrids. Realizing ultrastrong light-matter coupling in condensed matter systems has largely relied on bosonic matter modes. Here, the authors report ultrastrong coupling between a cavity photon mode and paramagnetic spins in gadolinium gallium garnet, consistent with the spin-boson physics described by the Dicke model.
Quantum electrodynamics lies at the heart of hybrid quantum systems essential for future technologies. The thermodynamic limit of the Dicke model, a fundamental model describing these systems, predicts exotic quantum phenomena, such as equilibrium superradiant phase transitions and ground-state two-mode squeezing. However, the experimental realization of genuine Dicke systems has remained elusive due to the inevitable existence of gauge-invariant self-interaction terms that hinder such phenomena. Here, we report on the on-chip realization of a Dicke-type system utilizing ultrastrong magnetic-dipole interactions between collective excitations in a spatially separated ferromagnetic array and a superconducting resonator, resulting in creation of magnon polaritons. Crucially, this spatially separated architecture allows the cooperative enhancement of the coupling strength without increasing the self-interaction energy. We experimentally confirm the Bloch-Siegert shift, originating from the counter-rotating terms, alongside the suppression of self-excitation terms required to observe critical Dicke physics. Our results establish a versatile platform, which provides the playground to explore quantum collective coupling physics and open pathways towards integrated quantum devices harnessing Dicke physics.
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.
Strong light-matter coupling gives rise to polaritons - hybrid excitations whose mixed photonic and matter character enables control over optical, electronic and chemical properties. This Feature Article surveys the main architectures supporting polariton formation, including photonic microcavities, plasmonic nanostructures, open cavities and metasurfaces, and outlines how inorganic semiconductors, organic aggregates and hybrid systems access strong and ultrastrong coupling. Key phenomena such as coherent dynamics, vibronic interactions, dark-state reservoirs and polariton-mediated energy and electron transport are discussed, together with the experimental and theoretical tools used to study them. We highlight examples where strong coupling modifies charge transport, energy flow and chemical reactivity, and we summarize emerging regimes, including intermediate and dark-strong coupling, that broaden the landscape of hybrid light-matter physics.
Present-day experiments have started to couple traditional simulations of ultracold atom experiments with quantum light-fields in cavities. This has provided a wealth of op- portunities to enlarge the number of interaction potentials: cavity mediated long-range interactions compete with kinetic energies, longitudinal fields, short-ranged collisional or magnetic spin-spin interactions. The intracavity many-body lattice models often have to be maintained far from equilibrium through the presence of external driving lasers that help to boost and engineer the various interaction potentials. The steady influx of energy is compensated by a steady stream of energy out of the atom-cavity system for example by photon losses or atomic spontaneous emission. Several experiments have demonstrated that such environments can give rise to new competing quantum phases. \nBut this long-standing ambition to push for models with tailorable interaction potentials can bring with it also considerable challenges in their theoretical description, since sponta- neous symmetry breaking transitions in many body lattice systems coupled to dynamical light-fields with single-photon character occur in the presence of drive and dissipation for the photonic force carriers. This clearly calls for model systems where the above men- tioned interplay of interactions, drive, dissipation and cooperative many-body behaviour can be theoretically studied to provide simple, experimentally verifiable predictions. \nThe Dicke model is, through its simplicity (an exactly solved ferromagnet with infinite range atom-atom interactions mediated by a single cavity mode), an exceptionally well- suited candidate. As the generic model for atom-light interactions, it has been experimen- tally realized in a variety of modern quantum optical systems, highlighting its relevance for present-day research. The Dicke model is also highly versatile itself. It has been extended into the dissipative realm, was promoted to account for multiple optical light modes and was used to describe multiple, coupled single-mode cavity structures. It was adapted to treat spin-selective coupling to a cavity to describe superradiance phase tran- sitions in multi-level atomic systems. Moreover, it was realised in electronic circuits where the dipole coupling of real atoms to single mode fields is replaced by a capacitive cou- pling of artificial atoms to a resonator mode. This illustrates that the Dicke model and its extended variants are ’future-proof’ and continue to be of relevance for fundamental light-matter interactions and for driven-dissipative phase transitions. \nIn this thesis, we investigate magnetic phase transitions in driven-dissipative atomic en- sembles interacting with quantum light. We present three research projects on variants of cooperative radiation of an ensemble of laser driven two-level atoms in a single mode optical cavity, as described by the Dicke model. \nThroughout the chapters 2,3 and 4 that contain the main body of research of this thesis, we investigate phase transitions between non-equilibrium stationary states in engineered quantum-optical systems each of which extends the conventional Dicke model physics. As a starting point, we map the quantum equations of motion onto a set of semiclassical nonlinear stochastic equations and analyse their stationary states and instabilities with master equations for atomic spin and photon mean-field amplitudes. These are used to obtain experimentally relevant parameters such as critical atom-light couplings for phase transitions, phase diagrams and properties of stationary non-equilibrium states in addition to cavity output spectra that identify the imprint of magnetic correlations in the light-field. \nIn chapter 2, we help resolve a discrepancy between earlier experimental investigations of the critical atom-light coupling strength for the superradiance transition in the Dicke model: higher external pumping strengths than theoretically predicted were needed to observe a coherent, superradiant state of the light field in an optical cavity. By including incoherent spontaneous emission of atomic excitations, we extend the dissipative Dicke model to a two loss channel variant containing both photon leakage and atomic decay that reproduces the experimentally observed critical atom-light coupling. \nRecent experiments have started to interface quantum many body lattice models with coherent cavity fields, thereby allowing to realize new quantum phases through competing atom-cavity and atom-atom interactions. In chapter 3, we consider a simplified model for such a set-up where a single quantized mode of the light-field interacts with an ensemble of Rydberg-dressed atoms inside a high finesse optical cavity. This model provides a base case for further studies of quantum magnets in optical cavities. At the heart of this model is a competition of short- (dipolar atom-atom) and long-range (atom-light) interactions at the Hamiltonian level in the presence of both spontaneous emission and photon leak- age through the cavity mirrors. We show that different magnetic phases can coexist with coherent atomic radiation and provide clear experimental signatures to identify the mag- netic structure and intra-cavity dynamics. We suggest an experimental level-scheme for a quantum optical implementation of our model. \nIn chapter 4 we consider a generic, collective decay for many-body excitations in the paradigmatic Dicke model. This extension drastically enriches the dynamics as it induces a bicritical point and a bistable regime dominated by true non-equilibrium fluctuations that induce a dissipative first-order phase transition that can only be resolved by including finite fluctuation corrections with the help of stochastic Langevin equations. We investigate the hysteretic response to time-dependent ramps of the atom-light coupling. Discontinuous first-order phase transitions where metastable states coexist in a hysteresis domain have been investigated in recent dissipative quantum-optical experiments. We review noise- activation far from thermal equilibrium in chapter 5.
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.