T. Elijah Kritzell, Jacques Doumani, Tobias Asano, Sota Yamada, Fuyang Tay, Hongjing Xu, Han Yan, Ikufumi Katayama, Jun Takeda, Andriy H. Nevidomskyy, Hiroyuki Nojiri, Motoaki Bamba, Andrey Baydin, Junichiro Kono
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.
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.
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.
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.
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.
Abstract The Dicke model describes the cooperative interaction of an ensemble of two-level atoms with a single-mode photonic field and exhibits a quantum phase transition as a function of light–matter coupling strength. Extending this model by incorporating short-range atom–atom interactions makes the problem intractable but is expected to produce new physical phenomena and phases. Here, we simulate such an extended Dicke model using a crystal of ErFeO 3 , where the role of atoms (photons) is played by Er 3+ spins (Fe 3+ magnons). Through terahertz spectroscopy and magnetocaloric effect measurements as a function of temperature and magnetic field, we demonstrated the existence of a novel atomically ordered phase in addition to the superradiant and normal phases that are expected from the standard Dicke model. Further, we elucidated the nature of the phase boundaries in the temperature–magnetic-field phase diagram, identifying both first-order and second-order phase transitions. These results lay the foundation for studying multiatomic quantum optics models using well-characterized many-body solid-state systems.
Strong coupling of light and matter is an essential element of cavity quantum electrodynamics (cavity-QED) and quantum optics, which may lead to novel mixed states of light and matter and to applications such as quantum computation. In the strong-coupling regime, where the coupling strength exceeds the dissipation, the light-matter interaction produces a characteristic vacuum Rabi splitting. Therefore, strong coupling can be utilized as an effective coherent interface between light and matter (in the form of electron charge, spin or superconducting Cooper pairs) to achieve components of quantum information technology including quantum memory, teleportation, and quantum repeaters. Semiconductor quantum dots, nuclear spins and paramagnetic spin systems are only some of the material systems under investigation for strong coupling in solid-state physics. Mixed states of light and matter coupled via electric dipole transitions often suffer from short coherence times (nanoseconds). Even though magnetic transitions appear to be intrinsically more quantum coherent than orbital transitions, their typical coupling strengths have been estimated to be much smaller. Hence, they have been neglected for the purposes of quantum information technology.\nHowever, we predict that strong coupling is feasible between photons and a ferromagnetic nanomagnet, due to exchange interactions that cause very large numbers of spins to coherently lock together with a significant increase in oscillator strength while still maintaining very long coherence times. In order to examine this new exciting possibility, the interaction of a ferromagnetic nanomagnet with a single photonic mode of a cavity is analyzed in a fully quantum-mechanical treatment. Exceptionally large quantum-coherent magnet-photon coupling with coupling terms in excess of several THz are predicted to be achievable in a spherical cavity of ∼ 1 mm radius with a nanomagnet of ∼ 100 nm radius and ferromagnet resonance frequency of ∼ 200 GHz. This should substantially exceed the coupling observed in solids between orbital transitions and light. Eigenstates of the nanomagnet-photon system correspond to entangled states of spin orientation and photon number over 105 values of each quantum number. Initial coherent state of definite spin and photon number evolve dynamically to produce large coherent oscillations in the microwave power with exceptionally long dephasing times of few seconds. In addition to dephasing, several decoherence mechanisms including elementary excitation of magnons and crystalline magnetic anisotropy are investigated and shown to not substantially affect coherence upto room temperature. For small nanomagnets the crystalline magnetic anisotropy of the magnet strongly localize the eigenstates in photon and spin number, quenching the potential for coherent states and for a sufficiently large nanomagnet the macrospin approximation breaks down and different domains of the nanomagnet may couple separately to the photonic mode. Thus the optimal nanomagnet size is predicted to be just below the threshold for failure of the macrospin approximation. Moreover, it is shown that initially unentangled coherent states of light (cavity field) and spin (nanomagnet spin orientation) can be phase-locked to evolve into a coherent entangled states of the system under the influence of strong coupling.