Quantum science and technology devices exploiting collective spins in thermal gases are extremely appealing due to their simplicity and robustness. This comes at the cost of dealing with the random thermal motion of the atoms which is usually an uncontrolled source of decoherence and noise. There are however conditions, for example, when diffusing in a buffer gas, where thermal atoms can occupy a discrete set of stable spatial modes. Diffusive modes can be extended or localized, have different magnetic properties depending on boundary conditions, and can react differently to external perturbations. Here, we selectively excite, manipulate, and interrogate the longest-lived of these modes by using laser light. In particular, we identify the conditions for the generation of modes that are exceptionally resilient to detrimental effects such as light induced frequency shifts and power-broadening, which are often the dominant sources of systematic errors in atomic magnetometers and comagnetometers. Moreover, we show that the presence of spatial inhomogeneities in the pump introduces a coupling that leads to a coherent exchange of excitation between the two longest-lived modes. Our results demonstrate that systematic engineering of the multi-mode nature of diffusive gases has great potential for improving the performance of quantum sensors based on alkali-metal thermal vapors, and opens new perspectives for quantum information applications. Published by the American Physical Society 2024
Quantum science and technology devices exploiting collective spins in thermal gases are extremely appealing due to their simplicity and robustness. This comes at the cost of dealing with the random thermal motion of the atoms which is usually an uncontrolled source of decoherence and noise. There are however conditions, for example, when diffusing in a buffer gas, where thermal atoms can occupy a discrete set of stable spatial modes. Diffusive modes can be extended or localized, have different magnetic properties depending on boundary conditions, and can react differently to external perturbations. Here, we selectively excite, manipulate, and interrogate the longest-lived of these modes by using laser light. In particular, we identify the conditions for the generation of modes that are exceptionally resilient to detrimental effects such as light induced frequency shifts and power-broadening, which are often the dominant sources of systematic errors in atomic magnetometers and comagnetometers. Moreover, we show that the presence of spatial inhomogeneities in the pump introduces a coupling that leads to a coherent exchange of excitation between the two longest-lived modes. Our results demonstrate that systematic engineering of the multi-mode nature of diffusive gases has great potential for improving the performance of quantum sensors based on alkali-metal thermal vapors, and opens new perspectives for quantum information applications. Published by the American Physical Society 2024
Lanthanides, like erbium and dysprosium, have emerged as powerful platforms for quantum-gas research due to their diverse properties, including a significant large spin manifold in their absolute ground state. However, effectively exploiting the spin richness necessitates precise manipulation of spin populations, a challenge yet to be fully addressed in this class of atomic species. In this work, we present an all-optical method for deterministically controlling the spin composition of a dipolar bosonic erbium gas, based on a clocklike transition in the telecom window at 1299 n m . The atoms can be prepared in just a few tens of microseconds in any spin-state composition using a sequence of Rabi-pulse pairs, selectively coupling Zeeman sublevels of the ground state with those of the long-lived clocklike state. Finally, we demonstrate that this transition can also be used to create spin-selective light shifts, thus fully suppressing spin-exchange collisions. These experimental results unlock exciting possibilities for implementing advanced spin models in isolated, clean, and fully controllable lattice systems. Published by the American Physical Society 2024
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.
A form of quantum control is proposed by applying twisted light, also known as optical vortex beams, to drive ultranarrow atomic transitions in neutral Ca, Mg, Yb, Sr, Hg, and Cd bosonic isotopes. This innovative all-optical spectroscopic method introduces spatially tailored electric and magnetic fields to fully rewrite atomic selection rules, reducing simultaneously probe-induced frequency shifts and additional action of external ac and dc field distortions. A twisted-light focused probe beam produces strong longitudinal electric and magnetic fields along the laser propagation axis, which opens the $^{1}S_{0}\ensuremath{\rightarrow}^{3}P_{0}$ doubly forbidden clock transition with a high E1M1 two-photon excitation rate. This long-lived clock transition is thus immune to nonscalar electromagnetic perturbations. Zeeman components of the M2 magnetic quadrupole $^{1}S_{0}\ensuremath{\rightarrow}^{3}P_{2}$ transition considered for quantum computation and simulation are now selectively driven by transverse or longitudinal field gradients with vanishing electric fields. These field gradients are manipulated by the mutual action of orbital and spin angular momentum of the light beam and are used in presence of tunable vector and tensor polarizabilities. A combination of these two different twisted-light induced clock transitions within a single quantum system, at the same magic wavelength and in presence of a common thermal environment, significantly reduces systematic uncertainties. Furthermore, it generates an optical synthetic frequency which efficiently limits the blackbody radiation shift and its variations at room temperature. Engineering light-matter interaction by optical vortices merged with composite pulses will ultimately benefit experimental atomic and molecular platforms targeting an optimal coherent control of quantum states, reliant quantum simulation, novel approaches to atomic interferometry, and precision tests of fundamental theories in physics and high-accuracy optical metrology.
Experimental platforms based on ultracold atomic gases have significantly advanced the quantum simulation of complex systems, yet the exploration of phenomena driven by long-range interactions remains a formidable challenge. Currently available methods utilizing dipolar quantum gases or multimode cavities allow us to implement long-range interactions with a 1 / r 3 character or with a spatial profile fixed by the mode structure of the vacuum electromagnetic field surrounding the atoms, respectively. Here, we propose an experimental scheme employing laser-painted cavity-mediated interactions, which enables the realization of atom-atom interactions that are fully tunable in range, shape, and sign. Our approach combines the versatility of cavity quantum electrodynamics with the precision of laser manipulation, thus providing a highly flexible platform for simulating and understanding long-range interactions in quantum many-body systems. Our analytical predictions are supported by numerical simulations describing the full dynamics of the atoms, the laser, and the cavity. These reveal the self-organization of domains in the density of the atomic cloud, confirming the finite-range nature of the induced interactions. We demonstrate that there is a wide and experimentally accessible parameter regime in which our protocol works robustly, with negligible heating of the quantum gas. The methodology not only paves the way for exploring new territories in quantum simulation but also enhances the understanding of fundamental physics, potentially leading to the discovery of novel quantum states and phases. Published by the American Physical Society 2024
We present a comprehensive theory of nuclear spin polarization of 3He and 129Xe gases by spin-exchange collisions with optically pumped alkali-metal vapors. The most important physical processes considered are (1) spin-conserving spin-exchange collisions between like or unlike alkali-metal atoms; (2) spin-destroying collisions of the alkali-metal atoms with each other and with buffer-gas atoms; (3) electron-nuclear spin-exchange collisions between alkali-metal atoms and 3He or 129Xe atoms; (4) spin interactions in van der Waals molecules consisting of a Xe atom bound to an alkali-metal atom; (5) optical pumping by laser photons; (6) spatial diffusion. The static magnetic field is assumed to be small enough that the nuclear spin of the alkali-metal atom is well coupled to the electron spin and the total spin is very nearly a good quantum number. Conditions appropriate for the production of large quantities of spin-polarized 3He or 129Xe gas are assumed, namely, atmospheres of gas pressure and nearly complete quenching of the optically excited alkali-metal atoms by collisions with N2 or H2 gas. Some of the more important results of this work are as follows: (1) Most of the pumping and relaxation processes are sudden with respect to the nuclear polarization. Consequently, the steady-state population distribution of alkali-metal atoms is well described by a spin temperature, whether the rate of spin-exchange collisions between alkali-metal atoms is large or small compared to the optical pumping rate or the collisional spin-relaxation rates. (2) The population distributions that characterize the response to sudden changes in the intensity of the pumping light are not described by a spin temperature, except in the limit of very rapid spin exchange. (3) Expressions given for the radio-frequency (rf) resonance linewidths and areas can be used to make reliable estimates of the local spin polarization of the alkali-metal atoms. (4) Diffusion effects for these high-pressure conditions are mainly limited to thin layers at the cell surface and at internal resonant surfaces generated by radio-frequency magnetic fields when the static magnetic field has substantial spatial inhomogeneities. The highly localized effects of diffusion at these surfaces are described with closed-form analytic functions instead of the spatial eigenmode expansions that are appropriate for lower-pressure cells.
Motivated by rapid experimental progress in the fields of ultracold atoms and quantum optics, I present a series of theoretical studies which explore collective phenomena in quantum gases of atoms and photons. In Chapter 1, I highlight the major developments in the research field and identify the overarching themes and motivations. I also provide a roadmap for the rest of the thesis and summarize the main results. The remaining eight chapters contain original studies, organized along three broad motifs. In Chapters 2 through 5, I investigate how the nature of collective excitations and quasiparticles can be explored in modern experiments. More specifically, I model the dynamics of a spin impurity in a Bose lattice gas, develop a protocol for observing fractionalized excitations or anyons in an optical cavity, and characterize the collective dynamics of Bogoliubov quasiparticles and domain walls in a Fermi superfluid. In Chapters 6 and 7, I examine unconventional superfluid phases in spin-imbalanced Fermi gases. In particular, I propose a novel technique for engineering the long-sought-after Fulde-Ferrell-Larkin-Ovchinnikov (FFLO) phase and study the relative stability of exotic phases across a dimensional crossover. Finally, Chapters 8 and 9 are devoted to studies of kinetics in out-of-equilibrium systems. I model the formation of a Bose-Einstein condensate in a dimple trap and characterize the approach to thermal equilibrium in quasi-one-dimensional geometries.