Rydberg Gas Research Articles

Deexcitation spectroscopy of strongly interacting Rydberg gases

We present experimental results on the controlled de-excitation of Rydberg states in a cold gas of Rb atoms. The effect of the van der Waals interactions between the Rydberg atoms is clearly seen in the de-excitation spectrum and dynamics. Our observations are confirmed by numerical simulations. In particular, for off-resonant (facilitated) excitation we find that the de-excitation spectrum reflects the spatial arrangement of the atoms in the quasi one-dimensional geometry of our experiment. We discuss future applications of this technique and implications for detection and controlled dissipation schemes.

Epidemic Dynamics in Open Quantum Spin Systems.

We explore the nonequilibrium evolution and stationary states of an open many-body system that displays epidemic spreading dynamics in a classical and a quantum regime. Our study is motivated by recent experiments conducted in strongly interacting gases of highly excited Rydberg atoms where the facilitated excitation of Rydberg states competes with radiative decay. These systems approximately implement open quantum versions of models for population dynamics or disease spreading where species can be in a healthy, infected or immune state. We show that in a two-dimensional lattice, depending on the dominance of either classical or quantum effects, the system may display a different kind of nonequilibrium phase transition. We moreover discuss the observability of our findings in laser driven Rydberg gases with particular focus on the role of long-range interactions.

Velocity-selective spectroscopy measurements of Rydberg fine structure states in a hot vapor cell**Project supported by the National Natural Science Foundation of China (Grant Nos. 61475091 and 61227902), the National Key Research and Development Program of China (Grant No. 2017YFA0304502), and the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi, China (Grant No. 2017101).

A velocity-selective spectroscopy technique for studying the spectra of Rydberg gases is presented. This method provides high-resolution spectrum measurements. We present experimental results for a ladder system 6S1/2 → 6P3/2 →nS(D) electromagnetically-induced transparency involving highly-excited Rydberg states. Based on a radio-frequency modulation technique, we measure the hyperfine structure splitting of intermediate states and the fine structure splitting of Rydberg states in a room temperature 133Cs vapor cell. The experimental data and theoretical predictions show excellent agreement.

Creation and detection of photonic molecules in Rydberg gases

We consider the propagation of photons in a gas of Rydberg atoms under conditions of electromagnetically induced transparency, where they form strongly interacting massive particles, termed Rydberg polaritons. Depending on the strength of the van der Waals-type interactions of the atoms either bunching or anti-bunching of photons can be observed when driving the atoms off-resonantly. The bunching is associated with the formation of bound states. We employ a Green's function approach and numerical wave-function simulations to analyze the conditions for the creation and the dynamics of these photonic molecules and their interplay with the scattering continuum which can also show photon bunching. Analytic solutions of the pair-propagation problem obtained from a pseudopotential approximation and verified numerically provide a detailed understanding of bound and scattering states. We find that the scattering contributions acquire asymptotically a robust relative phase which can be employed to separate bound-state and scattering contributions by a homodyne detection scheme.

Arrested relaxation in an isolated molecular ultracold plasma

Spontaneous avalanche to plasma splits the core of an ellipsoidal Rydberg gas of nitric oxide. Ambipolar expansion first quenches the electron temperature of this core plasma. Then, long-range, resonant charge transfer from ballistic ions to frozen Rydberg molecules in the wings of the ellipsoid quenches the centre-of-mass ion/Rydberg molecule velocity distribution. This sequence of steps gives rise to a remarkable mechanics of self-assembly, in which the kinetic energy of initially formed hot electrons and ions drives an observed separation of plasma volumes. These dynamics adiabatically sequester energy in a reservoir of mass transport, starting a process that anneals separating volumes to form an apparent glass of strongly coupled ions and electrons. Short-time electron spectroscopy provides experimental evidence for complete ionization. The long lifetime of this system, particularly its stability with respect to recombination and neutral dissociation, suggests that this transformation affords a robust state of arrested relaxation, far from thermal equilibrium.

Lévy statistics of interacting Rydberg gases

A statistical analysis of the laser excitation of cold and randomly distributed atoms to Rydberg states is developed. We first demonstrate with a hard ball model that the distribution of energy level shifts in an interacting gas obeys L\'evy statistics, in any dimension $d$ and for any interaction $-C_p/R^p$ under the condition $d/p<1$. This result is confirmed with a Monte Carlo rate equations simulation of the actual laser excitation in the particular case $p=6$ and $d=3$. With this finding, we develop a statistical approach for the modeling of probe light transmission through a cold atom gas driven under conditions of electromagnetically induced transparency involving a Rydberg state. The simulated results are in good agreement with experiment.

Multicritical behavior in dissipative Ising models.

We analyze theoretically the many-body dynamics of a dissipative Ising model in a transverse field using a variational approach. We find that the steady-state phase diagram is substantially modified compared to its equilibrium counterpart, including the appearance of a multicritical point belonging to a different universality class. Building on our variational analysis, we establish a field-theoretical treatment corresponding to a dissipative variant of a Ginzburg-Landau theory, which allows us to compute the upper critical dimension of the system. Finally, we present a possible experimental realization of the dissipative Ising model using ultracold Rydberg gases.

Emergent equilibrium in many-body optical bistability.

Many-body systems constructed of quantum-optical building blocks can now be realized in experimental platforms ranging from exciton-polariton fluids to ultracold Rydberg gases, establishing a fascinating interface between traditional many-body physics and the driven-dissipative, nonequilibrium setting of cavity QED. At this interface, the standard techniques and intuitions of both fields are called into question, obscuring issues as fundamental as the role of fluctuations, dimensionality, and symmetry on the nature of collective behavior and phase transitions. Here, we study the driven-dissipative Bose-Hubbard model, a minimal description of numerous atomic, optical, and solid-state systems in which particle loss is countered by coherent driving. Despite being a lattice version of optical bistability, a foundational and patently nonequilibrium model of cavity QED, the steady state possesses an emergent equilibrium description in terms of a classical Ising model. We establish this picture by making new connections between traditional techniques from many-body physics (functional integrals) and quantum optics (the system-size expansion). To lowest order in a controlled expansion-organized around the experimentally relevant limit of weak interactions-the full quantum dynamics reduces to nonequilibrium Langevin equations, which support a phase transition described by model A of the Hohenberg-Halperin classification. Numerical simulations of the Langevin equations corroborate this picture, revealing that canonical behavior associated with the Ising model manifests readily in simple experimental observables.

Anomalous excitation facilitation in inhomogeneously broadened Rydberg gases

When atomic gases are laser driven to Rydberg states in an off resonant way, a single Rydberg atom may enhance the excitation rate of surrounding atoms. This leads to a facilitated excitation referred to as Rydberg anti-blockade. In the usual facilitation scenario, the detuning of the laser from resonance compensates the interaction shift. Here, we discuss a different excitation mechanism, which we call anomalous facilitation. This occurs on the "wrong side" of the resonance and originates from inhomogeneous broadening. The anomalous facilitation may be seen in experiments of attractively interacting atoms on the blue detuned side, where facilitation is not expected to appear.

Quantum signature for laser-driven correlated excitation of Rydberg atoms

The excitation dynamics of a laser-driven Rydberg gas exhibits a cooperative effect due to the interatomic Rydberg-Rydberg interaction, but the large many-body system with inhomogeneous Rydberg coupling is hard to exactly solved or numerically study by density matrix equations. In this paper, we find that the laser-driven Rydberg gas with most of the atoms being in the ground state can be described by a simplified interaction model resembling the optical Kerr effect if the distance-dependent Rydberg-Rydberg interaction is replaced by an infinite-range coupling. We can then quantitatively study the effect of the quantum fluctuations on the Rydberg excitation with the interatomic correlation involved and analytically calculate the statistical characteristics of the excitation dynamics in the steady state, revealing the quantum signature of the driven-dissipative Rydberg gas. The results obtained here will be of great interest for other spin-1/2 systems with spin-spin coupling.

Radiation trapping in a dense cold Rydberg gas

Cold atomic gases resonantly excited to Rydberg states can exhibit strong optical nonlinearity at the single photon level. We observe that in such samples radiation trapping leads to an additional mechanism for Rydberg excitation. Conversely we demonstrate that Rydberg excitation provides a novel in situ probe of the spectral, statistical, temporal and spatial properties of the trapped re-scattered light. We also show that absorption can lead to an excitation saturation that mimics the Rydberg blockade effect. Collective effects due to multiple scattering may co-exist with co-operative effects due to long-range interactions between the Rydberg atoms, adding a new dimension to quantum optics experiments with cold Rydberg gases.

Autler-Townes splitting of ultracold cesium Rydberg atoms

Autler-Townes (A-T) splitting, known as an AC Stark effect, shows a change of an absorption/emission spectral line of a probe beam when an oscillating field is tuned in resonance with the atomic or molecular transition. The A-T splitting is observed in different three-level atoms and widely investigated in a vapor cell and in a magneto-optical trap (MOT). The A-T splitting plays an important role in the atom-based microwave electric-field measurements where a cascade three-level system involving Rydberg state is adopted. In this work, an A-T splitting is observed in an ultracold cesium Rydberg gas, which is cooled down to about 100 pK and center density is about 1010 cm-3 in a conventional MOT by using the laser cooling technology. We present the A-T spectrum in a ladder three-level atomic system involving a 34D5/2 Rydberg state. The cesium ground state (6S1/2), excited state (6P3/2) and Rydberg state (34D5/2) constitute a Rydberg three-level system. A coupling laser, locked to the Rydberg transition by using a Rydberg electromagnetically induced transparency signal that is obtained from a cesium room-temperature vapor cell, couples 6P3/2 (F'=5) 34D5/2 Rydberg transition. A weak probe laser, stabilized to a ground-state transition by using a polarization spectroscopy, is swept, covering the transition 6S1/2 (F=4) 6P3/2 (F'=5) with a double-passed acousto-optic modulator. The probe and coupling lasers are counter-propagated through the MOT center. The power of probe light is 200 pW, corresponding Rabi frequency p=21.05 MHz. During the experiment, 50 s after turning off the trapping laser, both the coupling and probe beams are switched on and last 100 s. The A-T spectrum as a function of the probe detuning is detected with a single-photon counter module detector. We use Gaussian multiple peak fitting to obtain the positions of the A-T peaks and the A-T splitting. The measured A-T splitting is proportional to the Rabi frequency of the coupling light. We numerically solve the density matrix equations to obtain the A-T spectrum, and the calculations reproduce A-T spectra well. The measured A-T splitting shows good agreement with the theoretical calculation for Rabi frequency of the coupling light c29 MHz. The A-T splitting is less than the calculation for the case of c29 MHz, the deviation is mainly attributed to the increased dephasing rate induced by the strong interaction between Rydberg atoms, whose number increases with the coupling laser Rabi frequency. In this work, the adopted method for the cascade three-level system involving Rydberg state is also suitable for -and V-type cases.

Controlling the interactions between cold Rydberg atoms by a time-varying electric field

Long-range interactions between cold Rydberg atoms are being investigated for neutral-atom quantum computing, quantum simulations, phase transitions in cold Rydberg gases and other applications. Fine tuning of the interaction strength can be implemented using Förster resonances between Rydberg atoms controlled by an electric field. The observation of the Stark-tuned Förster resonances between Rydberg atoms excited by narrowband cw laser radiation requires usage of a Stark-switching technique in order to excite the atoms first in a fixed electric field and then to induce the interactions in a varied electric field, which is scanned across the Förster resonance. The application of the radio-frequency field causes additional Förster resonances between collective states, whose line shape depends on the interaction strengths and time. Spatial averaging over the atom positions in a single interaction volume yields a cusped line shape of the Förster resonance. We present a detailed experimental and theoretical analysis of the line shape and time dynamics of the Stark-tuned Förster resonances Rb(nP3/2) + Rb(nP3/2) → Rb(nS1/2) + Rb([n + 1]S1/2) for two Rb Rydberg atoms interacting in a time-varying electric field.

Near-field measurements of the even-order harmonics undetectable in far-field measurements

Even-order harmonics (EOHs) are generated for oriented molecules and for atoms under specific conditions. Here, we focus on the most common situations where EOHs are not observed in far-field measurements. We propose an experiment to show that the EOHs are produced close to the nucleus but are not detected in the far-field measurements due to destructive interferences of the propagated EOHs of the emitted radiation. However, Rydberg gas atoms (e.g., rubidium), which are out of the focus of the laser beam, are expected to be ionized due to their weak interaction with a specific EOH of helium, which is not observed by the far-field detector. The ionization energy of the Rydberg gas atoms should be in resonance with the single-photon energy of a specific EOH.

Long-range Rydberg molecules, Rydberg macrodimers and Rydberg aggregates in an ultracold Cs gas

We present an overview of our recent investigations of long-range interactions in an ultracold Cs Rydberg gas. These interactions are studied by high-resolution photoassociation spectroscopy, using excitation close to one-photon transitions into np3/2 Rydberg states with pulsed and continuous-wave ultraviolet laser radiation, and lead to the formation of long-range Cs2 molecules. We observe two types of molecular resonances. The first type originates from the correlated excitation of two atoms into Rydberg-atom-pair states interacting at long range via multipole-multipole interactions. The second type results from the interaction of one atom excited to a Rydberg state with one atom in the electronic ground state. Which type of resonances is observed in the experiments depends on the laser intensity and frequency and on the pulse sequences used to prepare the Rydberg states. We obtain insights into both types of molecular resonances by modelling the interaction potentials, using a multipole expansion of the long-range interaction for the first type of resonances and a Fermi-contact pseudo-potential for the second type of resonances. We analyse the relation of these long-range molecular resonances to molecular Rydberg states and ion-pair states, and discuss their decay channels into atomic and molecular ions. In experiments carried out with a two-colour two-photon excitation scheme, we observe a large enhancement of Rydberg-excitation probability, which we interpret as a saturable autocatalytic antiblockade phenomenon.

Few-body interactions in frozen Rydberg gases

The strong dipole-dipole coupling and the Stark tunability make Forster resonances an attractive tool for the implementation of quantum gates. In this direction a generalization to a N-body process would be a powerful instrument to implement multi-qubit gate and it will also path the way to the understanding of many-body physics. In this review, we give a general introduction on Forster resonances, also known as two-body FRET, giving an overview of the different application in quantum engineering and quantum simulation. Then we will describe an analogous process, the quasi-forbidden FRET, which is related to the Stark mixing due to the presence of an external electric field. We will then focus on its use in a peculiar four-body FRET. The second part of this review is focused on our study of few-body interactions in a cold gas of Cs Rydberg atoms. After a detailed description of a series of quasi-forbidden resonances detected in the proximity of an allowed two-body FRET we will show our most promising result: the observation of a three-body FRET. This process corresponds to a generalization of the usual two-body FRET, where a third atom serves as a relay for the energy transport. This relay also compensates for the energy mismatch which prevents a direct two-body FRET between the donor and the acceptor, but on the other side allowed a three-body process; for this reason, the three-body FRET observed is a “Borromean” process. It can be generalized for any quantum system displaying two-body FRET from quasi-degenerate levels. We also predict N-body FRET, based on the same interaction scheme. Three-body FRET thus promises important applications in the formation of macro-trimers, implementation of few-body quantum gates, few-body entanglement or heralded entanglement.

Mean-field energy-level shifts and dielectric properties of strongly polarized Rydberg gases

Mean-field energy-level shifts arising as a result of strong electrostatic dipole interactions within dilute gases of polarized helium Rydberg atoms have been probed by microwave spectroscopy. The Rydberg states studied had principal quantum numbers $n=70$ and 72, and electric dipole moments of up to 14050 D, and were prepared in pulsed supersonic beams at particle number densities on the order of $10^{8}$ cm$^{-3}$. Comparisons of the experimental data with the results of Monte Carlo calculations highlight effects of the distribution of nearest-neighbor spacings in the pulsed supersonic beams, and the dielectric properties of the strongly polarized Rydberg gases, on the microwave spectra. These observations reflect the emergence of macroscopic electrical properties of the atomic samples when strongly polarized.

Direct observation of ultrafast many-body electron dynamics in an ultracold Rydberg gas.

Many-body correlations govern a variety of important quantum phenomena such as the emergence of superconductivity and magnetism. Understanding quantum many-body systems is thus one of the central goals of modern sciences. Here we demonstrate an experimental approach towards this goal by utilizing an ultracold Rydberg gas generated with a broadband picosecond laser pulse. We follow the ultrafast evolution of its electronic coherence by time-domain Ramsey interferometry with attosecond precision. The observed electronic coherence shows an ultrafast oscillation with a period of 1 femtosecond, whose phase shift on the attosecond timescale is consistent with many-body correlations among Rydberg atoms beyond mean-field approximations. This coherent and ultrafast many-body dynamics is actively controlled by tuning the orbital size and population of the Rydberg state, as well as the mean atomic distance. Our approach will offer a versatile platform to observe and manipulate non-equilibrium dynamics of quantum many-body systems on the ultrafast timescale.

Thermodynamic of mixtures of ultracold Rydberg gases with different levels of excitation

The physical model of the particle system describing the thermodynamics of mixtures of ultracold Rydberg gases with different levels of excitation are proposed. In our model system of particles is a mixture of atoms in S-state and atoms in the P-state. To calculate the thermodynamic of the mixture Rydberg gases the method of Monte-Carlo was used. Computational results of the spatial correlations of dipoles depending on the coupling parameter are presented. At some value of the nonideality parameter the dipole chains are formed.

Spectral shift and dephasing of electromagnetically induced transparency in an interacting Rydberg gas

We perform spectroscopic measurements of electromagnetically induced transparency (EIT) in a strongly interacting Rydberg gas, and observe a significant spectral shift of the transparency from the single-atom EIT resonance as well as a spectral dephasing of the same order. We characterize the shift and dephasing as a function of atomic density, probe Rabi frequency, and principal quantum number of Rydberg states, and demonstrate that the observed spectral shift and dephasing are reduced if the size of a Gaussian atomic cloud is increased. We simulate our experiment with a semi-analytical model, which gives results in good agreement with our experimental data.