Quantum Dynamics of Kerr Optical Frequency Combs below and above Threshold: Spontaneous Four-Wave-Mixing, Entanglement and Squeezed States of Light

In this article, we use quantum Langevin equations to provide a theoretical understanding of the non-classical behavior of Kerr optical frequency combs when pumped below and above threshold. In the configuration where the system is under threshold, the pump field is the unique oscillating mode inside the resonator, and triggers the phenomenon of spontaneous four-wave mixing, where two photons from the pump are symmetrically up- and down-converted in the Fourier domain. This phenomenon can only be understood and analyzed from a fully quantum perspective as a consequence of the coupling between the field of the central (pumped) mode and the vacuum fluctuations of the various sidemodes. We analytically calculate the power spectra of the spontaneous emission noise, and we show that these spectra can be either single- or double peaked depending on the parameters of the system. We also calculate as well the overall spontaneous noise power per sidemode, and propose simplified analytical expressions for some particular cases. In the configuration where the system is pumped above threshold, we investigate the phenomena of quantum correlations and multimode squeezed states of light that can occur in the Kerr frequency combs originating from stimulated four-wave mixing. We show that for all stationary spatio-temporal patterns, the side-modes that are symmetrical relatively to the pumped mode in the frequency domain display quantum correlations that can lead to squeezed states of light. We also explicitly determine the phase quadratures leading to photon entanglement, and analytically calculate their quantum noise spectra. We finally discuss the relevance of Kerr combs for quantum information systems at optical telecommunication wavelengths, below and above threshold.Comment: 27 pages, 11 figure

Nonequilibrium Dynamics in Open Quantum Systems

Due to the variety of tools available to control atomic, molecular, and optical (AMO) systems, they provide a versatile platform for studying many-body physics, quantum simulation, and quantum computation. Although extensive efforts are employed to reduce coupling between the system and the environment, the effects of the environment can never fully be avoided, so it is important to develop a comprehensive understanding of open quantum systems. The system-environment coupling often leads to loss via dissipation, which can be countered by a coherent drive. Open quantum systems subject to dissipation and drive are known as driven-dissipative systems, and they provide an excellent platform for studying many-body nonequilibrium physics. The first part of this dissertation will focus on driven-dissipative phase transitions. Despite the nonequilibrium nature of these systems, the corresponding phase transitions tend to exhibit emergent equilibrium behavior. However, we will show that in the vicinity of a multicritical point where multiple phase transitions intersect, genuinely nonequilibrium criticality can emerge, even though the individual phase transitions on their own exhibit equilibrium criticality. These nonequilibrium multicritical points can exhibit a variety of exotic phenomena not possible for their equilibrium counterparts, including the emergence of complex critical exponents, which lead to discrete scale invariance and spiraling phase boundaries. Furthermore, the Liouvillian gap can take on complex values, and the fluctuation-dissipation theorem is violated, corresponding to an effective temperature which gets "hotter" and "hotter" at longer and longer wavelengths. The second part of this dissertation will focus on Rydberg atoms. In particular, we study how the spontaneous generation of contaminant Rydberg states drastically modifies the behavior of a driven-dissipative Rydberg system due to the resultant dipole-dipole interactions. These interactions lead to a complicated competition of both blockade and anti-blockade effects, leading to strongly enhanced Rydberg populations for far-detuned drive and reduced Rydberg populations for resonant drive

Magnetic Phase Transitions in Driven-Dissipative Atomic Ensembles Interacting with Quantum Light

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. But 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. The 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. In 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. Throughout 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. In 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. Recent 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. In 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