We study theoretically and experimentally the competing blockade and antiblockade effects induced by spontaneously generated contaminant Rydberg atoms in driven Rydberg systems. These contaminant atoms provide a source of strong dipole-dipole interactions and play a crucial role in the system's behavior. We study this problem theoretically using two different approaches. The first is a cumulant expansion approximation, in which we ignore third-order and higher connected correlations. Using this approach for the case of resonant drive, a many-body blockade radius picture arises, and we find qualitative agreement with previous experimental results. We further predict that as the atomic density is increased, the Rydberg population's dependence on Rabi frequency will transition from quadratic to linear dependence at lower Rabi frequencies. We study this behavior experimentally by observing this crossover at two different atomic densities. We confirm that the larger density system has a smaller crossover Rabi frequency than the smaller density system. The second theoretical approach is a set of phenomenological inhomogeneous rate equations. We compare the results of our rate-equation model to the experimental observations [E. A. Goldschmidt et al., Phys. Rev. Lett. 116, 113001 (2016)] and find that these rate equations provide quantitatively good scaling behavior of the steady-state Rydberg population for both resonant and off-resonant drives.
We study theoretically and experimentally the competing blockade and antiblockade effects induced by spontaneously generated contaminant Rydberg atoms in driven Rydberg systems. These contaminant atoms provide a source of strong dipole-dipole interactions and play a crucial role in the system's behavior. We study this problem theoretically using two different approaches. The first is a cumulant expansion approximation, in which we ignore third-order and higher connected correlations. Using this approach for the case of resonant drive, a many-body blockade radius picture arises, and we find qualitative agreement with previous experimental results. We further predict that as the atomic density is increased, the Rydberg population's dependence on Rabi frequency will transition from quadratic to linear dependence at lower Rabi frequencies. We study this behavior experimentally by observing this crossover at two different atomic densities. We confirm that the larger density system has a smaller crossover Rabi frequency than the smaller density system. The second theoretical approach is a set of phenomenological inhomogeneous rate equations. We compare the results of our rate-equation model to the experimental observations [E. A. Goldschmidt et al., Phys. Rev. Lett. 116, 113001 (2016)] and find that these rate equations provide quantitatively good scaling behavior of the steady-state Rydberg population for both resonant and off-resonant drives.
Resonant laser excitation of multiple Rydberg atoms are prohibited, leading to Rydberg blockade, when the long-range van der Waals interactions are stronger than the laser-atom coupling. Rydberg blockade can be violated, i.e., simultaneous excitation of more than one Rydberg atom, by off-resonant laser excitation, causing an excitation antiblockade. Rydberg antiblockade gives rise to strongly correlated many-body dynamics and spin-orbit coupling and also finds quantum computation applications. Instead of commonly used van der Waals interactions, we investigate antiblockade dynamics of two Rydberg atoms interacting via dipole-dipole exchange interactions. We study typical situations in current Rydberg atom experiments, where different types of dipole-dipole interactions can be achieved by varying Rydberg state couplings. An effective Hamiltonian governing underlying antiblockade dynamics is derived. We illustrate that geometric gates can be realized with the Rydberg antiblockade which is robust against the decay of Rydberg states. Our study may stimulate new experimental and theoretical exploration of quantum optics and strongly interacting many-body dynamics with Rydberg antiblockade driven by dipole-dipole interactions.
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.
Interaction between Rydberg atoms can significantly modify Rydberg excitation dynamics. Under a resonant driving field the Rydberg-Rydberg interaction in high-lying states can induce shifts in the atomic resonance such that a secondary Rydberg excitation becomes unlikely leading to the Rydberg blockade effect. In a related effect, off-resonant coupling of light to Rydberg states of atoms contributes to the Rydberg anti-blockade effect where the Rydberg interaction creates a resonant condition that promotes a secondary excitation in a Rydberg atomic gas. Here, we study the light-matter interaction and dynamics of off-resonant two-photon excitations and include two- and three-atom Rydberg interactions and their effect on excited state dynamics in an ensemble of cold atoms. In an experimentally-motivated regime, we find the optimal physical parameters such as Rabi frequencies, two-photon detuning, and pump duration to achieve significant enhancement in the probability of generating doubly-excited collective atomic states. This results in large auto-correlation values due to the Rydberg anti-blockade effect and makes this system a potential candidate for a high-purity two-photon Fock state source.
In this thesis I present several theoretical methods to explore the excitation dynamics of Ultracold Rydberg systems in various regimes. For some applications the details of interactions between Rydberg atoms have to be carefully examined, while for others, the many-body aspect of Rydberg excitation may be crucial. In both cases, the basic prerequisite is to know the interactions sufficiently well. I will review the basic concepts how to evaluate molecular potentials in various Hund's cases and approximations. Long-range Rydberg-Rydberg interactions between Rydberg atoms induce ℓ-mixing which in certain situations gives rise to molecular resonances. For these resonances, we calculate long-range potentials in Hund's case (c) by diagonalization of an interaction matrix. The excitation dynamics of the resonances is always modeled as pair excitation. At high principal quantum number n, the interactions between Rydberg atoms can blockade the excitation of many surrounding atoms in the range of few μm. The atoms within this range are strongly correlated so that many-body treatments are, in general, needed. To describe this blockading effect and other manifestations of the collective behavior of Rydberg excitation, such as the many-body Rabi oscillations, spatial correlations between atoms and the fluctuations of the number of excited atoms, I have used three different approaches. In the mean-field approach the interactions between different atoms is modeled by a distribution of mean-field shifts for which a distribution of probabilities is calculated, A good agreement between the theoretical model and experimental measurements is found. To study the correlations between atoms the many-body wavefunction is numerically computed. The possibility of observing the many-body Rabi oscillations of Rydberg excitation and other aspects of many-body dynamics is analyzed. Although strong interactions cannot be treated perturbatively other expansions may be feasible. I will show that the expansion in powers of the single atom Rabi frequency can be evaluated in the interaction and Heisenberg picture. The expansion is expected to behave well for arbitrary strong interactions. ^
The work presented in this dissertation concerns dynamics of Rydberg atom lattices in the presence of noise and dissipation. Rydberg atoms possess a number of exaggerated properties, such as a strong van der Waals interaction. The interplay of that interaction, coherent driving and decoherence leads to intriguing non-equilibrium phenomena. Here, we study the non-equilibrium physics of driven atom lattices in the presence of decoherence caused by either laser phase noise or strong decay. In the first case, we compare between global and local noise and explore their effect on the number of excitations and the full counting statistics. We find that both types of noise give rise to a characteristic distribution of the Rydberg excitation number. The main method employed is the Langevin equation but for the sake of efficiency in certain regimes, we use a Markovian master equation and Monte Carlo rate equations, respectively. In the second case, we consider dissipative systems with more general power-law interactions. We determine the phase diagram in the steady state and analyse its generation dynamics using Monte Carlo rate equations. In contrast to nearest-neighbour models, there is no transition to long-range-ordered phases for realistic interactions and resonant driving. Yet, for finite laser detunings, we show that Rydberg atom lattices can undergo a dissipative phase transition to a long-range-ordered antiferromagnetic phase. We identify the advantages of Monte Carlo rate equations over mean field predictions. Having studied the dynamics of Rydberg atom lattices, we study an application of the strong interactions in such systems for quantum information processing. We investigate the coherent exchange of a single photon between a superconducting microwave cavity and a lattice of strongly interacting Rydberg atoms in the presence of local electric field fluctuations plaguing the cavity surface. We show that despite the increased sensitivity of Rydberg states to electric fields, as compared to ground state atoms, the Rydberg dipole-dipole interaction can be used to protect the system against the dephasing induced by the local noise. Using 1/f and laser phase noise models, we show that compared to the case with non-interacting atoms, our system exhibits longer coherence lifetimes and larger retrieval efficiency of the photon after storing into the atoms.
We study many-body correlations in the stationary state of a continuously driven, strongly interacting dissipative system. Specifically, we examine resonant optical excitations of Rydberg states of atoms interacting via long-range dipole-dipole and van der Waals potentials employing numerical and analytical techniques. Collection of atoms within a blockade distance form a ``superatom'' that can accommodate at most one Rydberg excitation. The superatom excitation probability saturates to 21 for coherently driven atoms but is significantly higher in the presence of dephasing, approaching unity as the number of atoms increases. Using the exact numerical solution of the density-matrix equations for a small system, we demonstrate that strong dephasing of the optically driven dipoles renders the many-body problem amenable to semiclassical Monte Carlo simulations. We employ the Monte Carlo algorithm for a large number of atoms and find that in the steady state of a uniformly driven, extended one-dimensional system, the saturation of superatoms leads to quasicrystallization of Rydberg excitations whose correlations exhibit damped spatial oscillations. We show that the behavior of the system under the van der Waals interaction potential can be approximated by a rate-equations model based on a ``hard-rod'' interatomic potential, and by solving it we obtain the period and correlation length for the density wave of Rydberg excitations.