We report clear evidence of the role of dipole-dipole interaction in Penning ionization of Rydberg atoms, leading to the formation of an ultracold plasma. Penning ionization of np Rydberg Cesium atoms is prevented for states with in n < 42, which correspond to a repulsive potential, but it does not occur for n larger than 42, corresponding to an attractive potential. Blackbody radiation is mostly responsible for the background and initial ionization, although ion-Rydberg collisions and population transfer due to limited superradiance may have to be considered.
We present a detailed analysis of our recent observation of synchronous Rabi oscillations between the electronic ground state and Rydberg states in a mesoscopic ensemble containing roughly 100 ultracold atoms [M. Reetz-Lamour \textit{et al.}, submitted, arXiv:0711.4321]. The mesoscopic cloud is selected out of a sample of laser-cooled Rb atoms by optical pumping. The atoms are coupled to a Rydberg state with principal quantum number around 30 by a two-photon scheme employing flat-top laser beams. The influence of residual spatial intensity fluctuations as well as sources of decoherence such as…
We present measurements on pulsed four-wave mixing involving a Rydberg state in an atomic vapor cell. The excitation to the Rydberg state is conducted by a pulsed two-photon excitation on the nanosecond timescale that is combined with a third CW laser in phase-matched geometry yielding light emission on the same timescale. An additional signal peak is observed shortly after the pulse that can be attributed to a revival of constructive interference between different velocity classes of the radiating atomic dipoles. Furthermore we investigate the density dependence of the four-wave mixing signal…
The results of a theoretical investigation of prompt many-body ionization are reported. Our calculations address an experiment that reported ionization in Rydberg gases for densities two orders of magnitude less than expected from ionization between pairs of atoms. The authors argued that the results were due to the simultaneous interaction between many atoms. We performed classical calculations for many interacting Rydberg atoms with the ions fixed in space and have found that the many atom interaction does allow ionization at lower densities than estimates from two atom interactions. However…
We demonstrate the coherent excitation of a mesoscopic ensemble of about 100 ultracold atoms to Rydberg states by driving Rabi oscillations from the atomic ground state. We employ a dedicated beam shaping and optical pumping scheme to compensate for the small transition matrix element. We study the excitation in a weakly interacting regime and in the regime of strong interactions. When increasing the interaction strength by pair state resonances we observe an increased excitation rate through coupling to high angular momentum states. This effect is in contrast to the proposed and previously ob…
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…
We report a quantum Monte Carlo calculation of the phase diagram of bosons interacting with a repulsive inverse sixth power pair potential, a model for assemblies of Rydberg atoms in the local van der Waals blockade regime. The model can be parametrized in terms of just two parameters, the reduced density and temperature. Solidification happens to the fcc phase. At zero temperature the transition density is found with the diffusion Monte Carlo method at density $ρ= 3.9 (\hbar^2/m C_6)^{3/4} $, where $C_6$ is the strength of the interaction. The solidification curve at non-zero temperature is s…
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…
A Rydberg and a ground-state atom can form ultralong range diatomic molecules provided the interaction between the ground-state atom and the Rydberg electron is attractive [C. H. Greene, et al., Phys. Rev. Lett. 85, 2458 (2000)]. A repulsive interaction does not support bound states. However, as we will show, adding a second ground-state atom, a bound triatomic molecule becomes possible constituting a Borromean Rydberg system.
The long-range dipole-dipole interaction can create delocalized states due to the exchange of excitation between Rydberg atoms. We show that even in a random gas many of the single-exciton eigenstates are surprisingly delocalized, composed of roughly one quarter of the participating atoms. We identify two different types of eigenstates: one which stems from strongly-interacting clusters, resulting in localized states, and one which extends over large delocalized networks of atoms. These two types of states can be excited and distinguished by appropriately tuned microwave pulses, and their rela…
Spectral line width broadening in Rydberg gases, a phenomenon previously attributed to the many-body effect, was observed experimentally almost a decade ago. The observed line width was typically 80-100 times larger than the average interaction strength predicted from a binary interaction. The interpretation of such a phenomenon is usually based on the so-called diffusion model, where the line width broadening mostly originates from the diffusion of excitations. In this paper, we present a model calculation to show that diffusion is not the main mechanism to the line width broadening. We find …
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…
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…
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…
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…
Long-range metastable molecules consisting of two cesium atoms in high Rydberg states have been observed in an ultracold gas. A sequential three-photon two-color photoassociation scheme was employed to form these molecules in states which correlate to $np(n+1)s$ dissociation asymptotes. Spectral signatures of bound molecular states are clearly resolved at the positions of avoided crossings between long-range van der Waals potential curves. The experimental results are in agreement with simulations based on a detailed model of the long-range multipole-multipole interactions of Rydberg-atom pair…
The devil's staircase is a fractal structure that characterizes the ground state of one-dimensional classical lattice gases with long-range repulsive convex interactions. Its plateaus mark regions of stability for specific filling fractions which are controlled by a chemical potential. Typically such staircase has an explicit particle-hole symmetry, i.e., the staircase at more than half-filling can be trivially extracted from the one at less than half filling by exchanging the roles of holes and particles. Here we introduce a quantum spin chain with competing short-range attractive and long-ra…
We demonstrate finite range binding potentials between pairs of Rydberg atoms interacting with each other via attractive and repulsive van der Waals potentials and driven by a microwave field. We show that, using destructive quantum interference to cancel single-atom Rydberg excitation, the Rydberg-dimer states can be selectively and coherently populated from the two-atom ground state. This can be used to realize a two-qubit interaction gate which is not susceptible to mechanical forces between the atoms and is therefore immune to motional decoherence.
Long ground-Rydberg coherence lifetime is interesting for implementing high-fidelity quantum logic gates, many-body physics, and other quantum information protocols. However, the potential formed by a conventional far-off-resonance red-detuned optical-dipole trap (ODT) is usually repulsive for Rydberg atoms, which will result in fast atom loss and low repetition rate of the experimental sequence. These issues can be addressed by a magic ODT. We performed the calculation of ODT's magic detuning for confinement of cesium ground state and Rydberg state with the same potential well. We used a sum-…
We describe a method for controlling many-body states in extended ensembles of Rydberg atoms, forming crystalline structures during laser excitation of a frozen atomic gas. Specifically, we predict the existence of an excitation number staircase in laser excitation of atomic ensembles into Rydberg states. Each step corresponds to a crystalline state with a well-defined of regularly spaced Rydberg atoms. We show that such states can be selectively excited by chirped laser pulses. Finally, we demonstarte that, sing quantum state transfer from atoms to light, such crystals can be used to create c…
Assemblies of Rydberg atoms subject to resonant dipole-dipole interactions form Frenkel excitons. We show that van-der-Waals shifts can significantly modify the exciton wave function, whenever atoms approach each other closely. As a result, attractive excitons and repulsive van-der-Waals interactions can be combined to form stable one-dimensional atom chains, akin to bound aggregates. Here the van-der-Waals shifts ensure a stronger homogeneous delocalisation of a single excitation over the whole chain, enabling it to bind up to six atoms. When brought into unstable configurations, such Rydberg…
Clouds of ultracold strontium 5s48s 1S0 or 5s47d 1D2 Rydberg atoms are created by two photon excitation of laser cooled 5s2 1S0 atoms. The spontaneous evolution of the cloud of low orbital angular momentum (low-l) Rydberg states towards an ultracold neutral plasma is observed by imaging resonant light scattered from core ions, a technique that provides both spatial and temporal resolution. Evolution is observed to be faster for the S-states, which display isotropic attractive interactions, than for the D-states, which exhibit anisotropic, principally repulsive interactions. Immersion of the at…
We study the repulsive van der Waals interaction of cold rubidium $70S_{1/2}$ Rydberg atoms by analysis of time-delayed pair correlation functions. After excitation, Rydberg atoms are allowed to accelerate under the influence of the van der Waals force. Their positions are then measured using a single-atom imaging technique. From the average pair correlation function of the atom positions we obtain the initial atom-pair separation and the terminal velocity, which yield the van der Waals interaction coefficient $C_{6}$. The measured $C_{6}$ value agrees well with calculations. The experimental …
We propose a method to realize the Frenkel-Kontorova model using an array of Rydberg dressed atoms. Our platform can be used to study this model with a range of realistic interatomic potentials. In particular, we concentrate on two types of interaction potentials: a springlike potential and a repulsive long-range potential. We numerically calculate the phase diagram for such systems and characterize the Aubry-like and commensurate-incommensurate phase transitions. Experimental realizations of this system that are possible to achieve using current technology are discussed.
We theoretically analyze the interactions and decay rates for atoms dressed by multiple laser fields to strongly interacting Rydberg states using a quantum master equation approach. In this framework a comparison of two-level and three-level Rydberg-dressing schemes is presented. We identify a resonant enhancement of the three-level dressed interaction strength which originates from cooperative multiphoton couplings as well as small distance dependent decay rates. In this regime the soft-core shape of the potential is independent of the sign of the bare Rydberg-Rydberg interaction, while its s…
We study the behavior of a Bose-Einstein condensate in which atoms are weakly coupled to a highly excited Rydberg state. Since the latter have very strong van der Waals interactions, this coupling induces effective, nonlocal interactions between the dressed ground state atoms, which, opposed to dipolar interactions, are isotropically repulsive. Yet, one finds partial attraction in momentum space, giving rise to a roton-maxon excitation spectrum and a transition to a supersolid state in three-dimensional condensates. A detailed analysis of decoherence and loss mechanisms suggests that these phe…
We investigate the spectral properties of a finite laser-driven lattice of ultracold Rydberg atoms exploiting the dipole blockade effect in the frozen Rydberg gas regime. Uniform one-dimensional lattices as well as lattices with variable spacings are considered. In the case of a weak laser coupling, we find a multitude of many-body Rydberg states with well-defined excitation properties which are adiabatically accessible starting from the ground state. A comprehensive analysis of the degeneracies of the spectrum as well as of the single and pair excitations numbers of the eigenstates is perform…
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…
We present the experimental demonstration of Rydberg blockade in thermal atomic vapor where the atoms are not necessarily be frozen. We show that not all the interacting atoms but only the atoms with same velocity collectively participate in the blockade process. Using this observation, we formulated a suitable model based on super atom picture to study blockade interaction in thermal vapor. We performed an experiment to measure Rydberg population in rubidium thermal vapor using optical heterodyne detection technique and density dependent suppression of Rydberg population is observed in suitab…
We show that microwave spectroscopy of a dense Rydberg gas trapped on a superconducting atom chip in the dipole blockade regime reveals directly the dipole-dipole many-body interaction energy spectrum. We use this method to investigate the expansion of the Rydberg cloud under the effect of repulsive van der Waals forces and the breakdown of the frozen gas approximation. This study opens a promising route for quantum simulation of many-body systems and quantum information transport in chains of strongly interacting Rydberg atoms.
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 experimentally demonstrate an original method to measure very accurately the density of a frozen Rydberg gas. It is based on the use of adiabatic transitions induced by the long-range dipole-dipole interaction in pairs of nearest neighbor Rydberg atoms by sweeping an electric field with time. The efficiency of this two-body process is experimentally tunable, depends strongly on the density of the gas and can be accurately calculated. The analysis of this efficiency leads to an accurate determination of the Rydberg gas density, and to a calibration of the Rydberg detection. Our method does n…
We discuss laser dressed dipolar and Van der Waals interactions between atoms and polar molecules, so that a cold atomic gas with laser admixed Rydberg levels acts as a designed reservoir for both elastic and inelastic collisional processes. The elastic scattering channel is characterized by large elastic scattering cross sections and repulsive shields to protect from close encounter collisions. In addition, we discuss a dissipative (inelastic) collision where a spontaneously emitted photon carries away (kinetic) energy of the collision partners, thus providing a significant energy loss in a s…
We report the sudden and spontaneous evolution of an initially correlated gas of repulsively interacting Rydberg atoms to an ultracold plasma. Under continuous laser coupling we create a Rydberg ensemble in the strong blockade regime, which at longer times undergoes an ionization avalanche. By combining optical imaging and ion detection, we access the full information on the dynamical evolution of the system, including the rapid increase in the number of ions and a sudden depletion of the Rydberg and ground state densities. Rydberg-Rydberg interactions are observed to strongly affect the dynam…
We present a method to model the interaction and the dynamics of atoms excited to Rydberg states. We show a way to solve the optical Bloch equations for laser excitation of the frozen gas in good agreement with the experiment. A second method, the Kinetic Monte Carlo method gives an exact solution of rate equations. Using a simple N-body integrator (Verlet), we are able to describe dynamical processes in space and time. Unlike more sophisticated methods, the Kinetic Monte Carlo simulation offers the possibility of numerically following the evolution of tens of thousands of atoms within a reaso…
We study a one-dimensional atomic lattice gas in which Rydberg atoms are excited by a laser and whose external dynamics is frozen. We identify a parameter regime in which the Hamiltonian is well-approximated by a spin Hamiltonian with quasi-local many-body interactions which possesses an exact analytic ground state solution. This state is a superposition of all states of the system that are compatible with an interaction induced constraint weighted by a fugacity. We perform a detailed analysis of this state which exhibits a cross-over between a paramagnetic phase with short-ranged correlations…
We study the quantum melting of quasi-one-dimensional lattice models in which the dominant energy scale is given by a repulsive dipolar interaction. By constructing an effective low-energy theory, we show that the melting of crystalline phases can occur into two distinct liquid phases, having the same algebraic decay of density-density correlations, but showing a different non-local correlation function expressing string order. We present possible experimental realizations using ultracold atoms and molecules, introducing an implementation based on resonantly driven Rydberg atoms that offers ad…
Arrays of Rydberg atoms constitute a highly tunable, strongly interacting venue for the pursuit of exotic states of matter. We develop a new strategy for accessing a family of fractionalized phases known as quantum spin liquids in two-dimensional Rydberg arrays. We specifically use effective field theory methods to study arrays assembled from Rydberg chains tuned to an Ising phase transition that famously hosts emergent fermions propagating within each chain. This highly entangled starting point allows us to naturally access spin liquids familiar from Kitaev's honeycomb model, albeit from an e…
The motion-induced dephasing is a severe problem that limits the accuracy of a quantum control process by using external laser fields in neutral Rydberg atoms. This dephasing is a major issue that limits the realizable fidelity of a quantum entangling gate with neutral atoms when there is a {\it gap} time for the Rydberg atom to drift freely. We find that such a dephasing can be largely suppressed by using a transition in a `V'-type dual-rail configuration. The left~(right) arm of this `V' represents a transition to a Rydberg state $|r_{1(2)}\rangle$ with a Rabi frequency $Ωe^{ikz}~(Ωe^{-ikz})…
We consider inter-atomic forces due to resonant dipole-dipole interactions within a dimer of highly excited Rydberg atoms, embedded in an ultra-cold gas. These forces rely on a coherent superposition of two-atom electronic states, which is destroyed by continuous monitoring of the dimer state through a detection scheme utilizing controllable interactions with the background gas atoms. We show that this intrinsic decoherence of the molecular energy surface can gradually deteriorate a repulsive dimer state, causing a mixing of attractive and repulsive character. For sufficiently strong decoheren…
Long ground-Rydberg coherence lifetime is interesting for implementing high-fidelity quantum logic gates, many-body physics, and other quantum information protocols. However, the potential well formed by a conventional far-off-resonance red-detuned optical-dipole trap that is attractive for ground-state cold atoms is usually repulsive for Rydberg atoms, which will result in the rapid loss of atoms and low repetition rate of the experimental sequence. Moreover, the coherence time will be sharply shortened due to the residual thermal motion of cold atoms. These issues can be addressed by a one-d…
