In a recent work [Phys. Rev. Lett. 98, 023004 (2007)] we have investigated the influence of attractive van der Waals interaction on the pair distribution and Penning ionization dynamics of ultracold Rydberg gases. Here we extend this description to atoms initially prepared in Rydberg states exhibiting repulsive interaction. We present calculations based on a Monte Carlo algorithm to simulate the dynamics of many atoms under the influence of both repulsive and attractive longrange interatomic forces. Redistribution to nearby states induced by black body radiation is taken into account, changing the effective interaction potentials. The model agrees with experimental observations, where the ionization rate is found to increase when the excitation laser is blue-detuned from the atomic resonance.
We develop an efficient Monte-Carlo approach to describe the optical response of cold three-level atoms in the presence of EIT and strong atomic interactions. In particular, we consider a "Rydberg-EIT medium" where one involved level is subject to large shifts due to strong van der Waals interactions with surrounding Rydberg atoms. We find excellent agreement with much more involved quantum calculations and demonstrate its applicability over a wide range of densities and interaction strengths. The calculations show that the nonlinear absorption due to Rydberg-Rydberg atom interactions exhibits…
We present time-resolved spectroscopic measurements of Rydberg-Rydberg interactions in an ultracold gas, revealing the pair dynamics induced by long-range van der Waals interactions between the atoms. By detuning the excitation laser, a specific pair distribution is prepared. Penning ionization on a microsecond timescale serves as a probe for the pair dynamics under the influence of the attractive long-range forces. Comparison with a Monte Carlo model not only explains all spectroscopic features but also gives quantitative information about the interaction potentials. The results imply that th…
Tailored quantum states of light can be created via a transfer of collective quantum states of matter to light modes. Such collective quantum states emerge in interacting many-body systems if thermal fluctuations are overcome by sufficient interaction strengths. Therefore, typically ultracold temperatures or strong confinement are required. We show that the exaggerated interactions between giant Rydberg atoms allow for collective quantum states even above room temperature. The emerging Rydberg blockade allows then only for a single Rydberg excitation. We experimentally implement a four-wave mi…
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 Lévy 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 …
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 dissipat…
We present quantum mechanical calculations of Auger decay rates for two Rubidium Rydberg atoms with weakly overlapping electron clouds. We neglect exchange effects and consider tensor products of independent atom states forming an approximate basis of the two-electron state space. We consider large sets of two-atom states with randomly chosen quantum numbers and find that the charge overlap between the two Rydberg electrons allows one to characterise the magnitude of the Auger decay rates. If the electron clouds overlap by more than one percent, the Auger decay rates increase approximately exp…
We experimentally investigate the nonlinear transmission spectrum of coherent light fields propagating through a Rydberg EIT medium with strong atomic interactions. In contrast to previous investigations, which have largely focused on resonant control fields, we explore here the full two-dimensional spectral response of the Rydberg gas. Our measurements confirm previously observed spectral features for a vanishing control-field detuning, but also reveal significant differences on two-photon resonance. In particular, we find qualitative deficiencies of mean-field models and rate-equation simula…
In excited molecules, the interaction between the covalent Rydberg and ion-pair channels forms a unique class of excited Rydberg states, in which the infinite manifold of vibrational levels are the equivalent of atomic Rydberg states with a heavy electron mass. Production of the ion pair states usually requires excitation through one or several interacting Rydberg states; these interacting channels are pathways for loss of flux, diminishing the rate of ion pair production. Here, we develop an analytical, asymptotic charge transfer model for the interaction between ultracold Rydberg molecular s…
We study electromagnetically induced transparency (EIT) of a weakly interacting cold Rydberg gas. We show that the onset of interactions is manifest as a depopulation of the Rydberg state and numerically model this effect by adding a density-dependent non-linear term to the optical Bloch equations. In the limit of a weak probe where the depopulation effect is negligible, we observe no evidence of interaction induced decoherence and obtain a narrow Rydberg dark resonance with a linewidth of <600 kHz, limited by the Rabi frequency of the coupling beam
We report the creation of an interacting cold Rydberg gas of strontium atoms. We show that the excitation spectrum of the inner valence electron is sensitive to the interactions in the Rydberg gas, even though they are mediated by the outer Rydberg electron. By studying the evolution of this spectrum we observe density-dependent population transfer to a state of higher angular momentum l. We determine the fraction of Rydberg atoms transferred, and identify the dominant transfer mechanism to be l-changing electron-Rydberg collisions associated with the formation of a cold plasma.
We review experimental and theoretical tools to excite, study and understand strongly interacting Rydberg gases. The focus lies on the excitation of dense ultracold atomic samples close to, or within quantum degeneracy, to high lying Rydberg states. The major part is dedicated to highly excited S-states of Rubidium, which feature an isotropic van-der-Waals potential. Nevertheless, the setup and the methods presented are also applicable to other atomic species used in the field of laser cooling and atom trapping.
We study the van der Waals interaction between Rydberg alkali-metal atoms with fine structure ($n^2L_j$; $L\leq 2$) and heteronuclear alkali-metal dimers in the ground rovibrational state ($X^1Σ^+$; $v=0$, $J=0$). We compute the associated $C_6$ dispersion coefficients of atom-molecule pairs involving $^{133}$Cs and $^{85}$Rb atoms interacting with KRb, LiCs, LiRb, and RbCs molecules. The obtained dispersion coefficients can be accurately fitted to a state-dependent polynomial $O(n^7)$ over the range of principal quantum numbers $40\leq n\leq 150$. For all atom-molecule pairs considered, Rydbe…
We theoretically investigate the effect of dissipation on multi-photon excitation of Rydberg atoms. The steady states and the dynamics are compared via two types of four-level excitation schemes with different dissipative paths of spontaneous emission. We find that in the case of strong Rydberg-Rydberg interaction, the schemes will settle in several different non-equilibrium steady states. The interesting aspect is that there exists the multi-stable steady states, which reveals the competition between interaction-induced nonlinearity and dissipation caused by spontaneous emission. A numerical …
The combination of high optical nonlinearity in the electromagnetically induced transparency (EIT) effect and strong electric dipole-dipole interaction (DDI) among the Rydberg-state atoms can lead to important applications in quantum information processing and many-body physics. One can utilize the Rydberg-EIT system in the strongly-interacting regime to mediate photon-photon interaction or qubit-qubit operation. One can also employ the Rydberg-EIT system in the weaklyinteracting regime to study the Bose-Einstein condensation of Rydberg polaritons. Most of the present theoretical models dealt …
We proposed utilizing a medium with a high optical depth (OD) and a Rydberg state of low principal quantum number, $n$, to create a weakly-interacting many-body system of Rydberg polaritons, based on the effect of electromagnetically induced transparency (EIT). We experimentally verified the mean field approach to weakly-interacting Rydberg polaritons, and observed the phase shift and attenuation induced by the dipole-dipole interaction (DDI). The DDI-induced phase shift or attenuation can be viewed as a consequence of the elastic or inelastic collisions among the Rydberg polaritons. Using a w…
We present an extension of our recent paper [Bienias et al., Phys. Rev. A 90, 053804 (2014)] in which we demonstrated the scattering properties and bound-state structure of two Rydberg polaritons, as well as the derivation of the effective low-energy many-body Hamiltonian. Here, we derive a microscopic Hamiltonian describing the propagation of Rydberg slow light polaritons in one dimension. We describe possible decoherence processes within a Master equation approach, and derive equations of motion in a Schroedinger picture by using an effective non-Hermitian Hamiltonian. We illustrate diagramm…
Finite-range interacting spin models are the simplest models to study the effect of beyond nearest-neighbour interactions and access new effects caused by the range of the interactions. Recent experiments have reached the regime of dominant interactions in Ising quantum magnets via optical coupling of trapped neutral atoms to Rydberg states. This approach allows for the tunability of all relevant terms in an Ising Hamiltonian with $1/r^6$ interactions in a transverse and longitudinal field. This review summarizes the recent progress of these implementations in Rydberg lattices with site-resolv…
Rate equation models are extensively used to describe the many-body states of laser driven atomic gases. We show that the properties of the rate equation model used to describe nonlinear optical effects arising in interacting Rydberg gases can be understood by considering the excitation of individual super-atoms. From this we deduce a simple semi-analytic model that accurately describes the Rydberg density and optical susceptibility for different dimensionalities. We identify the previously reported universal dependence of the susceptibility on the Rydberg excited fraction as an intrinsic prop…
We present a theoretical study on the system of laser-driven strongly interacting Rydberg atoms trapped in a two-dimensional triangular lattice, in which the dipole-dipole interactions between Rydberg states result in exotic quantum phases. By using the mean-field theory, we investigate the steady state solutions and analyze their dynamical stabilities. We find that in the strong-interaction limit, the dynamics of the system is chaotic and exhibits random oscillations under appropriate laser detunings. Lyapunov exponent criterion is introduced to confirm the existence of this chaotic behavior.…
We investigate a hybrid electro-mechanical system consisting of a pair of charged macroscopic mechanical oscillators coupled to a small ensemble of Rydberg atoms. The resonant dipole-dipole coupling between an internal atomic Rydberg transition and the mechanics allows cooling to its motional ground state with a single atom despite the considerable mass imbalance between the two subsystems. We show that the rich electronic spectrum of Rydberg atoms, combined with their high degree of optical control, paves the way towards implementing various quantum-control protocol for the mechanical oscilla…
We provide a theoretical framework describing slow-light polaritons interacting via atomic Rydberg states. We use a diagrammatic method to analytically derive the scattering properties of two polaritons. We identify parameter regimes where polariton-polariton interactions are repulsive. Furthermore, in the regime of attractive interactions, we identify multiple two-polariton bound states, calculate their dispersion, and study the resulting scattering resonances. Finally, the two-particle scattering properties allow us to derive the effective low-energy many-body Hamiltonian. This theoretical p…
We describe the emergence of strong spatial correlations, akin to liquid-like behavior and crystallization effects, in low (one and two) dimensional gases of cold Rydberg atoms. The presence of an external electric field permanently polarizes the atoms, which became highly correlated due to the long-range dipole-dipole interaction. We describe a theoretical approach particularly suited for strongly coupled systems and numerically obtain both the two-particle distribution function and the static structure factor. The experimental implementation of such highly interacting systems is discussed, i…
We theoretically investigate the dynamics of a gas of strongly interacting Rydberg atoms subject to a time-domain Ramsey interferometry protocol. The many-body dynamics is governed by an Ising-type Hamiltonian with long range interactions of tunable strength. We analyze and model the contrast degradation and phase accumulation of the Ramsey signal and identify scaling laws for varying interrogation times, ensemble densities, and ensemble dimensionalities.
Recent developments in the study of ultracold Rydberg gases demand an advanced level of experimental sophistication, in which high atomic and optical densities must be combined with excellent control of external fields and sensitive Rydberg atom detection. We describe a tailored experimental system used to produce and study Rydberg-interacting atoms excited from dense ultracold atomic gases. The experiment has been optimized for fast duty cycles using a high flux cold atom source and a three beam optical dipole trap. The latter enables tuning of the atomic density and temperature over several …
We investigate the effect of degenerate atomic states on the exciton delocalization of dipole-dipole interacting Rydberg assemblies. Using a frozen gas and regular one-, two-, and three-dimensional lattice arrangements as examples, we see that degeneracies can enhance the delocalization compared to the situation when there is no degeneracy. Using the Zeeman splitting provided by a magnetic field, we controllably lift the degeneracy to study in detail the transition between degenerate and non-degenerate regimes.
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…
Removing exactly one photon from an arbitrary input pulse is an elementary operation in quantum optics and enables applications in quantum information processing and quantum simulation. Here we demonstrate a deterministic single-photon absorber based on the saturation of an optically thick free-space medium by a single photon due to Rydberg blockade. Single-photon subtraction adds a new component to the Rydberg quantum optics toolbox, which already contains photonic logic building-blocks such as single-photon sources, switches, transistors, and conditional $π$-phase shifts. Our approach is sca…
We study electromagnetically induced transparency of a ladder type configuration in ultracold atomic gases, where the upper level is an electronically highly excited Rydberg state. The strong two-body interaction in the Rydberg state leads to the excitation blockade, where all but one atoms are shifted out of resonance such that the transmission of the probe light is affected. We show that molecular coupling in the Rydberg state causes an effective, two-body dephasing. The presence of the two-body dephasing leads to a similar blockade effect. Hence the overall blockade effect is enhanced by th…
In the combination of crossed electric and magnetic fields and the Coulomb field of the atomic nucleus the spectrum of the Rydberg electron in the vicinity of the Stark saddle-point are investigated at a quantum mechanical level. The results expose a quantum anomaly dissociation: quasibound states near and above the saddle-point ionization limit predicted at the semi-classical level disappear at a quantum mechanical level.
We analyze the ground state properties of a one-dimensional cold atomic system in a lattice, where Rydberg excitations are created by an external laser drive. In the classical limit, the ground state is characterized by a complete devil's staircase for the commensurate solid structures of Rydberg excitations. Using perturbation theory and a mapping onto an effective low energy Hamiltonian, we find a transition of these commensurate solids into a floating solid with algebraic correlations. For stronger quantum fluctuations the floating solid eventually melts within a second quantum phase transi…
We study dispersive optical nonlinearities of short pulses propagating in high number density, warm atomic vapors where the laser resonantly excites atoms to Rydberg $P$-states via a single-photon transition. Three different regimes of the light-atom interaction, dominated by either Doppler broadening, Rydberg atom interactions, or decay due to thermal collisions between groundstate and Rydberg atoms, are described. We show that using fast Rabi flopping and strong Rydberg atom interactions, both in the order of gigahertz, can overcome the Doppler effect as well as collisional decay, leading to…
Energy-conserving, angular momentum-changing collisions between protons and highly excited Rydberg hydrogen atoms are important for precise understanding of atomic recombination at the photon decoupling era, and the elemental abundance after primordial nucleosynthesis. Early approaches to $\ell$-changing collisions used perturbation theory for only dipole-allowed ($Δ\ell=\pm 1$) transitions. An exact non-perturbative quantum mechanical treatment is possible, but it comes at computational cost for highly excited Rydberg states. In this note we show how to obtain a semi-classical limit that is a…
The non-equilibrium dynamics of a gas of cold atoms in which Rydberg states are off-resonantly excited is studied in the presence of noise. The interplay between interaction and off-resonant excitation leads to an initial dynamics where aggregates of excited Rydberg atoms slowly nucleate and grow, eventually reaching long-lived meta-stable arrangements which then relax further on much longer timescales. This growth dynamics is governed by an effective Master equation which permits a transparent and largely analytical understanding of the underlying physics. By means of extensive numerical simu…
We consider two clouds of ground state alkali atoms in two distinct hyperfine ground states. Each level is far off-resonantly coupled to a Rydberg state, which leads to dressed ground states with a weak admixture of the Rydberg state properties. Due to this admixture, for a proper choice of the Rydberg states, the atoms experience resonant dipole-dipole interactions that induce mechanical forces acting on all atoms within both clouds. This behavior is in contrast to the dynamics predicted for bare dipole-dipole interactions between Rydberg superatoms, where only a single atom per cloud is subj…
High resolution laser Stark excitation of np (60 < n < 85) Rydberg states of ultra-cold cesium atoms shows an efficient blockade of the excitation attributed to long-range dipole-dipole interaction. The dipole blockade effect is observed as a quenching of the Rydberg excitation depending on the value of the dipole moment induced by the external electric field. Effects of eventual ions which could match the dipole blockade effect are discussed in detail but are ruled out for our experimental conditions. Analytic and Monte-Carlo simulations of the excitation of an ensemble of interacting Rydberg…
We show that the dipole-dipole interaction between three identical Rydberg atoms can give rise to bound trimer states. The microscopic origin of these states is fundamentally different from Efimov physics. Two stable trimer configurations exist where the atoms form the vertices of an equilateral triangle in a plane perpendicular to a static electric field. The triangle edge length typically exceeds $R\approx 2\,μ\text{m}$, and each configuration is two-fold degenerate due to Kramers' degeneracy. The depth of the potential wells and the triangle edge length can be controlled by external paramet…
Three-body Förster resonances at long-range interactions of Rydberg atoms were first predicted and observed in Cs Rydberg atoms by R.Faoro et al., Nature Comm. 6, 8173 (2015). In these resonances, one of the atoms carries away an energy excess preventing the two-body resonance, leading thus to a Borromean type of Förster energy transfer. But they were in fact observed as the average signal for the large number of atoms $N\gg1$. In this Letter we report on the first experimental observation of the three-body Förster resonances ${\rm 3}\times nP_{3/2} (|{\rm M}|)\to nS_{1/2} +(n+1)S_{1/2} +nP_{3…
When Rydberg states are excited in a dense atomic gas the mean number of excited atoms reaches a stationary value after an initial transient period. We shed light on the origin of this steady state that emerges from a purely coherent evolution of a closed system. To this end we consider a one-dimensional ring lattice, and employ the perfect blockade model, i.e. the simultaneous excitation of Rydberg atoms occupying neighboring sites is forbidden. We derive an equation of motion which governs the system's evolution in excitation number space. This equation possesses a steady state which is stro…
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 inte…
The scaling of the number of Rydberg excitations in a laser-driven cloud of atoms with the interaction strength is found to be affected by the finite size of the system. The scaling predicted by a theoretical model is compared with results extracted from a numerical many-body simulation. We find that the numerically obtained scaling exponent in general does not agree with the analytical prediction. By individually testing the assumptions leading to the theoretical prediction using the results from the numerical analysis, we identify the origin of the deviations, and explain it as arising from …
Interfacing light and matter at the quantum level is at the heart of modern atomic and optical physics and enables new quantum technologies involving the manipulation of single photons and atoms. A prototypical atom-light interface is electromagnetically induced transparency, in which quantum interference gives rise to hybrid states of photons and atoms called dark-state polaritons. We have observed individual dark-state polaritons as they propagate through an ultracold atomic gas involving Rydberg states. Strong long-range interactions between Rydberg atoms give rise to an effective interacti…
Using time-resolved measurements, we demonstrate coherent collective Rydberg excitation crossing over into Rydberg blockade in a dense and ultracold gas trapped at a distance of 100 $μ$m from a room-temperature atom chip. We perform Ramsey-type measurements to characterize the coherence. The experimental data are in good agreement with numerical results from a master equation using a mean-field approximation, and with results from a super-atom-based Hamiltonian. These results represent significant progress in exploring a strongly interacting driven Rydberg gas on an atom chip.
We show that the dipole-dipole interaction between two Rydberg atoms can lead to substantial Abelian and non-Abelian gauge fields acting on the relative motion of the two atoms. We demonstrate how the gauge fields can be evaluated by numerical techniques. In the case of adiabatic motion in a single internal state, we show that the gauge fields give rise to a magnetic field that results in a Zeeman splitting of the rotational states. In particular, the ground state of a molecular potential well is given by the first excited rotational state. We find that our system realises a synthetic spin-orb…
We study a system of atoms that are laser-driven to $nD_{3/2}$ Rydberg states and assess how accurately they can be mapped onto spin-$1/2$ particles for the quantum simulation of anisotropic Ising magnets. Using non-perturbative calculations of the pair interaction potentials between two atoms in the presence of both electric and magnetic fields, we emphasize the importance of a careful selection of the experimental parameters in order to maintain the Rydberg blockade and avoid excitation of unwanted Rydberg states. We then benchmark these theoretical observations against experiments using two…
The laser-excitation of Rydberg atoms in ultracold gases is often described assuming that the atomic motion is frozen during the excitation time. We show that this frozen gas approximation can break down for atoms that are held in optical lattices or microtraps. In particular, we show that the excitation dynamics is in general strongly affected by mechanical forces among the Rydberg atoms as well as the spread of the atomic wavepacket in the confining potential. This causes decoherence in the excitation dynamics - resulting in a dissipative blockade effect - that renders the Rydberg excitation…
Mean-field Pulse Adaptation for the Circularization of Interacting Rydberg Atoms
Forschungszentrum Jülich GmbH（于利希研究中心）；Institute for Theoretical Physics, University of Cologne（科隆大学理论物理研究所）；Dipartimento di Fisica e Astronomia, Università di Bologna（博洛尼亚大学物理与天文系）；OIST Graduate University（冲绳科学技术大学院大学）
Abstract Far-from equilibrium dynamics that lead to self-organization are highly relevant to complex dynamical systems not only in physics, but also in life-, earth-, and social sciences. It is challenging however to find systems with sufficiently controllable parameters that allow quantitatively modelling of emergent properties. Here, we study a non-equilibrium phase transition and observe signatures of self-organized criticality in a dilute thermal vapour of atoms optically excited to strongly interacting Rydberg states. Electromagnetically induced transparency (EIT) provides excellent contr…
