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 driven under conditions of electromagnetically induced transparency involving a Rydberg state. The simulated results are in good agreement with experiment.
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…
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…
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…
We investigate the phenomenon of bistability in a thermal gas of cesium atoms excited to Rydberg states. We present both measurements and a numerical model of the phenomena based on collisions. By directly measuring the plasma frequency, we show that the origin of the bistable behavior lies in the creation of a plasma formed by ionized Rydberg atoms. Recombination of ions and electrons manifests as fluorescence which allows us to characterize the plasma properties and study the transient dynamics of the hysteresis that occurs. We determine scaling parameters for the point of plasma formation, …
The specific kind of diffusion stimulated (rather than suppressed) by the external magnetic field, which was predicted for the first time by Schmelcher and Cederbaum in 1992, is considered here for the case of high-angular-momentum (i.e., approximately "circular") Rydberg atoms. The coefficient of such diffusion was calculated by a purely analytical approach and was found to be well relevant to the experiments on antihydrogen formation.
We report an experimental investigation of the facilitated excitation dynamics in off-resonantly driven Rydberg gases by separating the initial off-resonant excitation phase from the facilitation phase, in which successive facilitation events lead to excitation avalanches. We achieve this by creating a controlled number of initial seed excitations. Greater insight into the avalanche mechanism is obtained from an analysis of the full counting distributions. We also present simple mathematical models and numerical simulations of the excitation avalanches that agree well with our experimental res…
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…
Assemblies of highly excited Rydberg atoms in an ultracold gas can be set into motion by a combination of van-der-Waals and resonant dipole-dipole interactions. Thereby, the collective electronic Rydberg state might change due to non-adiabatic transitions, in particular if the configuration encounters a conical interaction. For the experimentally most accessible scenario, in which the Rydberg atoms are initially randomly excited in a three-dimensional bulk gas under blockade conditions, we numerically show that non-adiabatic transitions can be common when starting from the most energetic repul…
Photoexcitation rates for creation of ultralong-range Rydberg molecules (ULRM) with 31$\lesssim n \lesssim41$ in both ground and excited vibrational levels in cold ($T\sim900$~nK) gases of polarized and unpolarized $^{87}$Sr are presented. The measured production rates of the $ν=0, 1$ and 2 vibrational levels reveal rather different $n$ dependences which are analyzed by evaluating the Franck-Condon factors associated with excitation of the different vibrational levels and molecular rotational states. In particular, for gases of spin-polarized fermions, only Rydberg dimers with odd rotational q…
Cold, dense Rydberg gases produced in a cold-atom trap are investigated using spectroscopic methods and time-resolved electron counting. On the discrete Rydberg resonances we observe large trap losses and long lasting electron emission from the Rydberg gas (>30ms). Our observations are explained by quasi-elastic l-mixing collisions between Rydberg atoms and slow electrons that lead to the population of long-lived high-angular-momentum Rydberg states. These atoms thermally ionize slowly and with large probabilities, leading to the observed effects.
We present a comprehensive study of the diverse properties of heteronuclear Rydberg molecules, placing a special emphasis on those composed of the light alkali atoms, Li, Na, and K. Electron-atom scattering phase shifts, which determine the strength of the molecular bond, are calculated at very low energy and then used in a spin-dependent theoretical model to calculate accurate Rydberg molecule potential energy curves. The wide parameter range accessible by combining the various properties of different alkali atoms often leads to hybridized electronic states accessible via one or two photon ex…
We investigate the possibility of a bistable phase in an open many-body system. To this end we discuss the microscopic dynamics of a continuously off-resonantly driven Rydberg lattice gas in the regime of strong decoherence. Our experimental results reveal a prolongation of the temporal correlations with respect to the lifetime of a single Rydberg excitation and show strong evidence for the formation of finite-sized Rydberg excitation clusters in the steady state. We simulate our data using a simplified and a full many-body rate-equation model. The results are compatible with the formation of …
We discuss the density shift and broadening of Rydberg spectra measured in cold, dense atom clouds in the context of Rydberg atom spectroscopy done at room temperature, dating back to the experiments of Amaldi and Segrè in 1934. We discuss the theory first developed in 1934 by Fermi to model the mean-field density shift and subsequent developments of the theoretical understanding since then. In particular, we present a model whereby the density shift is calculated using a microscopic model in which the configurations of the perturber atoms within the Rydberg orbit are considered. We present sp…
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…
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.
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 show that cold Rydberg gases enable an efficient six-wave mixing process where terahertz or microwave fields are coherently converted into optical fields and vice versa. This process is made possible by the long lifetime of Rydberg states, the strong coupling of millimeter waves to Rydberg transitions and by a quantum interference effect related to electromagnetically induced transparency (EIT). Our frequency conversion scheme applies to a broad spectrum of millimeter waves due to the abundance of transitions within the Rydberg manifold, and we discuss two possible implementations based on …
Recent experiments have demonstrated the spontaneous evolution of a gas of ultracold Rydberg atoms into an expanding ultracold plasma, as well as the reverse process of plasma recombination into highly excited atomic states. Treating the evolution of the plasma on the basis of kinetic equations, while ionization/excitation and recombination are incorporated using rate equations, we have investigated theoretically the Rydberg-to-plasma transition. Including the influence of spatial correlations on the plasma dynamics in an approximate way we find that ionic correlations change the results only …
We present photo-excitation of ultra-long-range Rydberg molecules as a probe of spatial correlations in quantum gases. Rydberg molecules can be created with well-defined internuclear spacing, set by the radius of the outer lobe of the Rydberg electron wavefunction $R_n$. By varying the principal quantum number $n$ of the target Rydberg state, the molecular excitation rate can be used to map the pair-correlation function of the trapped gas $g^{(2)}(R_n)$. We demonstrate this with ultracold Sr gases and probe pair-separation length scales ranging from $R_n = 1400 - 3200$ $a_0$, which are on the …
Cold Rydberg atoms exposed to strong magnetic fields possess unique properties which open the pathway for an intriguing many-body dynamics taking place in Rydberg gases consisting of either matter or anti-matter systems. We review both the foundations and recent developments of the field in the cold and ultracold regime where trapping and cooling of Rydberg atoms have become possible. Exotic states of moving Rydberg atoms such as giant dipole states are discussed in detail, including their formation mechanisms in a strongly magnetized cold plasma. Inhomogeneous field configurations influence t…
We study a two-dimensional lattice gas of atoms that are photo-excited to high-lying Rydberg states in which they interact via the van-der-Waals interaction. We explore the regime of dominant nearest neighbor interaction where this system is intimately connected to a quantum version of Baxter's hard squares model. We show that the strongly correlated ground state of the Rydberg gas can be analytically described by a projected entangled pair state that constitutes the ground state of the quantum hard squares model. This correspondence allows us to identify a first order phase boundary where the…
We study the non-equilibrium steady state arising from the interplay between coherent and dissipative dynamics in strongly interacting Rydberg gases using a recently introduced variational method [H. Weimer, Phys. Rev. Lett. 114, 040402 (2015)]. We give a detailed discussion of the properties of this novel approach, and we provide a comparison with methods related to the Bogoliubov-Born-Green-Kirkwood-Yvon hierarchy. We find that the variational approach offers some intrinsic advantages, and we also show that it is able to explain the experimental results obtained in an ultracold Rydberg gas o…
We propose a novel scheme to efficiently tune the scattering length of two colliding ground-state atoms by off-resonantly coupling the scattering-state to an excited Rydberg-molecular state using laser light. For the s-wave scattering of two colliding ${^{87}}\mathrm{Rb}$ atoms, we demonstrate that the effective optical length and pole strength of this Rydberg optical Feshbach resonance can be tuned over several orders of magnitude, while incoherent processes and losses are minimised. Given the ubiquity of Rydberg molecular states, this technique should be generally applicable to homo-nuclear …
We have investigated formation of structures of Rydberg atoms excited from a disordered gas of ultracold atoms, using rate equations for two-photon Rydberg excitation in a single atom without eliminating the intermediate state. We have explored the validity range of these rate equations and defined a simple measure to determine, whether our model is applicable for a given set of laser parameters. We have applied these rate equations in Monte Carlo simulations of ultracold gases, for different laser beam profiles, and compared these simulations to experimental observations and find a general ag…
We have studied the associative ionization of a Rydberg atom and a ground state atom in an ultracold Rydberg gas. The measured scattering cross section is three orders of magnitude larger than the geometrical size of the produced molecule. This giant enhancement of the reaction kinetics is due to an efficient directed mass transport which is mediated by the Rydberg electron. We also find that the total inelastic scattering cross section is given by the geometrical size of the Rydberg electron's wavefunction.
We present an analytical theory for the nonlinear optical response of a strongly interacting Rydberg gas under conditions of electromagnetically induced transparency. Simple formulae for the third order optical susceptibility are derived and shown to be in excellent agreement with recent experiments. The obtained expressions reveal strong nonlinearities, which in addition are of highly nonlocal character. This property together with enormous strength of the Rydberg-induced nonlinearities is shown to yield a unique laboratory platform for nonlinear wave phenomena, such as collapse-arrested modu…
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 study trapped ions that are immersed in an ultracold gas of Rydberg-dressed atoms. By off-resonant coupling on a dipole-forbidden transition, the adiabatic atom-ion potential can be made repulsive. We study the energy exchange between the atoms and a single trapped ion and find that Langevin collisions are inhibited in the ultracold regime for these repulsive interactions. Therefore, the proposed system avoids recently observed ion heating in hybrid atom-ion systems caused by coupling to the ion's radio frequency trapping field and retains ultracold temperatures even in the pr…
Dense Rydberg gases are out-of-equilibrium systems where strong density-density interactions give rise to effective kinetic constraints. They cause dynamic arrest associated with highly-constrained many-body configurations, leading to slow relaxation and glassy behavior. Multi-component Rydberg gases feature additional long-range interactions such as excitation-exchange. These are analogous to particle swaps used to artificially accelerate relaxation in simulations of atomistic models of classical glass formers. In Rydberg gases, however, swaps are real physical processes, which provide dynami…
Two-dimensional (2D) spectroscopy uses multiple electromagnetic pulses to infer the properties of a complex system. A paradigmatic class of target systems are molecular aggregates, for which one can obtain information on the eigenstates, various types of static and dynamic disorder and on relaxation processes. However, two-dimensional spectra can be difficult to interpret without precise knowledge of how the signal components relate to microscopic Hamiltonian parameters and system-bath interactions. Here we show that two-dimensional spectroscopy can be mapped in the microwave domain to highly …
The creation of collective many-body quantum states from a two-dimensional lattice gas of atoms is studied. Our approach relies on the van-der-Waals interaction that is present between alkali metal atoms when laser excited to high-lying Rydberg s-states. We focus on a regime in which the laser driving is strong compared to the interaction between Rydberg atoms. Here energetically low-lying many-particle states can be calculated approximately from a quadratic Hamiltonian. The potential usefulness of these states as a resource for the creation of deterministic single-photon sources is illustrate…
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…
We measure nonlocal third-order spatial correlations in non-degenerate ultracold gases of bosonic ($^{84}$Sr) and spin-polarized fermionic ($^{87}$Sr) strontium through studies of the formation rates for ultralong-range trimer Rydberg molecules. The trimer production rate is observed to be very sensitive to the effects of quantum statistics with a strong enhancement of up to a factor of six (3!) in the case of bosonic $^{84}$Sr due to bunching, and a marked reduction for spin-polarized fermionic $^{87}$Sr due to anti-bunching. The experimental results are compared to theoretical predictions an…
We show that the excitation of long-range Rydberg molecules in a three-dimensional optical lattice can be used as a position- and time-sensitive probe of the site occupancy in the system. To this end, we detect the ions which are continuously generated by the decay of the formed Rydberg molecules. While a superfluid gas shows molecule formation for all parameters, a Mott insulator with $n=1$ filling reveals a strong suppression of the number of formed molecules. In the limit of weak probing, the technique can be used to probe the superfluid to Mott-insulator transition in real-time. Our method…
Atoms excited into high-lying Rydberg states and under strong dipole-dipole interactions exhibit phenomena associated with highly correlated and complex systems. We perform first principles numerical simulations on the dynamics of such systems. The emergence of a roton minimum in the excitation spectrum, as expected in strongly correlated gases and accurately described by Feynman's theory of liquid helium, is shown to significantly inhibit particle transport, with a strong suppression of the diffusion coefficient, due to the emerging spatial order. We also demonstrate how the ability to tempor…
The spectral structure underlying excitonic energy transfer in ultra-cold Rydberg gases is studied numerically, in the framework of random matrix theory, and via self-consistent diagrammatic techniques. Rydberg gases are made up of randomly distributed, highly polarizable atoms that interact via strong dipolar forces. Dynamics in such a system is fundamentally different from cases in which the interactions are of short range, and is ultimately determined by the spectral and eigenvector structure. In the energy levels' spacing statistics, we find evidence for a critical energy that separates de…
A model for the simulation of ensembles of laser-driven Rydberg-Rydberg interacting multi-level atoms is discussed. Our hybrid approach combines an exact two-body treatment of nearby atom pairs with an effective approximate treatment for spatially separated pairs. We propose an optimized evolution equation based only on the system steady state, and a time-independent Monte Carlo technique is used to efficiently determine this steady state. The hybrid model predicts features in the pair correlation function arising from multi-atom processes which existing models can only partially reproduce. Ou…
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 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…
We report on the behaviour of the ionization avalanche in an ensemble of ultracold 87Rb atoms coupled to a high lying Rydberg state and investigate extensions to the current model by including the effects of three-body recombination and plasma expansion. To separate the two effects we study the time dependence of the plasma formation at various densities as well as for different nS and nD states. At medium densities and low n we observe the onset of the avalanche as has been reported in other experiments, as well as a subsequent turn-off of the avalanche for longer excitation times, which we a…
We study steady state phases of a one-dimensional array of Rydberg atoms coupled by a microwave (MW) field where the higher energy Rydberg state decays to the lower energy one via single-body and collective (superradiant) decay. Using mean-field approaches, we examine the interplay among the MW coupling, intra-state van der Waals (vdW) interaction, and single-body and collective dissipation between Rydberg states. A linear stability analysis reveals that a series of phases, including uniform, antiferromagnetic, oscillatory, and bistable and multistable phases can be obtained. Without the vdW i…
We observe the shift of Rydberg levels of rubidium close to a copper surface when atomic clouds are repeatedly deposited on it. We measure transition frequencies of rubidium to S and D Rydberg states with principal quantum numbers n between 31 and 48 using the technique of electromagnetically induced transparency. The spectroscopic measurement shows a strong increase of electric fields towards the surface that evolves with the deposition of atoms. Starting with a clean surface, we measure the evolution of electrostatic fields in the range between 30 and 300 \mum from the surface. We find that …
As was recently shown in Ref. 1, many eigenstates of a random Rydberg gas with resonant dipole-dipole interactions are highly delocalized. Although the high degree of delocalization is generic to various types of power-law interactions and to both two and three-dimensional systems, in their detailed aspects the coherence distributions are sensitive to these parameters and vary dramatically between different systems. We calculate the eigenstates of both two and three-dimensional gases and quantify their delocalization throughout the atoms in the gas using a coherence measure. By contrasting the…
We study the out-of-equilibrium dynamics of dissipative gases of atoms excited to two or more high-lying Rydberg states. This situation bears interesting similarities to classical binary (in general $p$-ary) mixtures of particles. The effective forces between the components are determined by the inter-level and intra-level interactions of Rydberg atoms. These systems permit to explore new parameter regimes which are physically inaccessible in a classical setting, for example one in which the mixtures exhibit non-additive interactions. In this situation the out-of-equilibrium evolution is chara…
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 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 …
We investigate the out-of-equilibrium behavior of a dissipative gas of Rydberg atoms that features a dynamical transition between two stationary states characterized by different excitation densities. We determine the structure and properties of the phase diagram and identify the universality class of the transition, both for the statics and the dynamics. We show that the proper dynamical order parameter is in fact not the excitation density and find evidence that the dynamical transition is in the "model A" universality class, i.e. it features a non-trivial $\mathbb{Z}_2$ symmetry and a dynam…
We investigate the evolution of interacting Rydberg gases in the limit of strong noise and dissipation. Starting from a description in terms of a Markovian quantum master equation we derive effective equations of motion that govern the dynamics on a "coarse-grained" timescale where fast dissipative degrees of freedom have been adiabatically eliminated. Specifically, we consider two scenarios which are of relevance for current theoretical and experimental studies --- Rydberg atoms in a two-level (spin) approximation subject to strong dephasing noise as well as Rydberg atoms under so-called elec…
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…
We calculate pair potential curves for interacting Rydberg atoms in a constant electric field and use them to determine the effective $C_3$ dipole-dipole and $C_6$ van der Waals coefficients. We compare the $C_3$ and $C_6$ with experiments where the angle of a polarizing electric field is varied with respect to the axis of a quasi-1-dimensional trap at ultracold temperatures. The dipoles produced via polarization of the atoms have an angular dependent dipole-dipole interaction. We focus on the interaction potential of two rubidium Rydberg atoms in $50S_{1/2}$ states in the blockade regime. For…
In the presence of strong dephasing noise the dynamics of Rydberg gases becomes effectively classical, due to the rapid decay of quantum superpositions between atomic levels. Recently a great deal of attention has been devoted to the stochastic dynamics that emerges in that limit, revealing several interesting features, including kinetically-constrained glassy behaviour, self-similarity and aggregation effects. However, the non-equilibrium physics of these systems, in particular in the regime where coherent and dissipative processes contribute on equal footing, is yet far from being understood…
We show that the dynamics of a laser driven Rydberg gas in the limit of strong dephasing is described by a master equation with manifest kinetic constraints. The equilibrium state of the system is uncorrelated but the constraints in the dynamics lead to spatially correlated collective relaxation reminiscent of glasses. We study and quantify the evolution towards equilibrium in one and two dimensions, and analyze how the degree of glassiness and the relaxation time are controlled by the interaction strength between Rydberg atoms. We also find that spontaneous decay of Rydberg excitations leads …
We investigate a possible mechanism for the autoionization of ultracold Rydberg gases, based on the resonant coupling of Rydberg pair states to the ionization continuum. Unlike an atomic collision where the wave functions begin to overlap, the mechanism considered here involves only the long-range dipole interaction and is in principle possible in a static system. It is related to the process of intermolecular Coulombic decay (ICD). In addition, we include the interaction-induced motion of the atoms and the effect of multi-particle systems in this work. We find that the probability for this io…