Within a dense environment (ρ ≈ 10 14 atoms=cm 3 ) at ultracold temperatures (T < 1 μK), a single atom excited to a Rydberg state acts as a reaction center for surrounding neutral atoms.At these temperatures, almost all neutral atoms within the Rydberg orbit are bound to the Rydberg core and interact with the Rydberg atom.We have studied the reaction rate and products for nS 87 Rb Rydberg states, and we mainly observe a state change of the Rydberg electron to a high orbital angular momentum l, with the released energy being converted into kinetic energy of the Rydberg atom.Unexpectedly, the measurements show a threshold behavior at n ≈ 100 for the inelastic collision time leading to increased lifetimes of the Rydberg state independent of the densities investigated.Even at very high densities (ρ ≈ 4.8 × 10 14 cm -3 ), the lifetime of a Rydberg atom exceeds 10 μs at n > 140 compared to 1 μs at n ¼ 90.In addition, a second observed reaction mechanism, namely, Rb þ 2 molecule formation, was studied.Both reaction products are equally probable for n ¼ 40, but the fraction of Rb þ 2 created drops to below 10% for n ≥ 90.
The lifetimes and decay channels of ultralong-range Rydberg molecules created in a dense Bose-Einstein condensate (BEC) are examined by monitoring the time evolution of the Rydberg population using field ionization. The Rydberg molecules, which contain tens to hundreds of ground state atoms within the electron orbit, have lifetimes of ∼ 1 to 5 µ s, their destruction being attributed to two main processes: formation of ions through associative ionization, and dissociation induced through L -changing reactions. The observed loss rates are consistent with a reaction model that emphasizes the interaction between the Rydberg core ion and its nearest neighbor ground state atom. The application of this model to earlier measurements of strontium dimer lifetimes at lower densities is discussed.
Atoms in highly excited Rydberg states possess physical characteristics quite unlike those associated with atoms in the ground or low-lying excited states. In particular, they are physically very large and are only very weakly bound. In consequence, collisions can lead to a wide variety of reaction processes many of which are unique to Rydberg species and have very large collision cross sections. In collisions with neutral targets, Rydberg atoms behave not as an atom but rather as a pair of well-separated independent scatterers, namely the core ion and the excited Rydberg electron. In the present article we discuss many of the different reactions that can occur when Rydberg atoms collide with neutral targets, focusing principally on reactions that are dominated by (binary) Rydberg electron-target interactions and include collisions with molecules that attach free low-energy electrons and with polar targets. In certain situations, however, interactions involving the Rydberg core ion are important. This is illustrated using as an example the destruction of ultralong-range Rydberg molecules excited in a cold dense gas.
A single Rydberg excitation in the high-density and low-temperature environment of a Bose-Einstein condensate (BEC) leads to a fascinating testbed of low-energy electron-neutral and ion-neutral scattering. In particular the small interparticle spacing in a BEC makes it possible to study the role of ion-neutral interactions in l-changing collisions on time scales much shorter than the Rydberg lifetime. We take advantage of the mean field density shift, caused by elastic electron-neutral collisions, to probe density dependent shells of the
87Rb BEC and thereby measure the l-changing collision time versus density and principal quantum number. We report on l-changing collisions due to inelastic scattering of the Rydberg electron with a neutral atom located near the Rydberg ionic core. We measure timescales of both the l-changing collision and the Rb
2 molecule formation of less than one microsecond for n
< 100 at the highest BEC densities. We extract a change in kinetic energy of the Rydberg atoms that matches well with the energy gap to the next-lowest manifold. We measure Rb
2 signal that decreases with increasing principal quantum number. The mechanism and timescales of the l-changing collision are compared with simulations including the motion of the ionic core and neutral atoms, as well as the Rydberg electron.
The lifetimes and decay channels of ultralong-range Rydberg molecules created in a dense Bose-Einstein condensate are examined by monitoring the time evolution of the Rydberg population using field ionization. Studies of molecules with values of the principal quantum number,
n, in the range
n=49 to
n=72 that contain tens to hundreds of ground-state atoms within the Rydberg electron orbit show that their presence leads to marked changes in the field ionization characteristics. The Rydberg molecules have lifetimes of $\ensuremath{\sim}1\ensuremath{-}5\phantom{\rule{0.16em}{0ex}}\ensuremath{\mu}\mathrm{s}$, their destruction being attributed to two main processes: formation of
Sr2+ ions through associative ionization and dissociation induced through
L-changing collisions. The observed loss rates are consistent with a reaction model that emphasizes the interaction between the Rydberg core ion and its nearest-neighbor ground-state atom. The measured lifetimes place strict limits on the time scales over which studies involving Rydberg species in cold, dense atomic gases can be undertaken and limit the coherence times for such measurements.
Combining ultracold atomic gases with the peculiar properties of Rydberg excited atoms gained a lot of theoretical and experimental attention in recent years. Embedded in the ultracold gas, an interaction between the Rydberg atom and the surrounding ground state atoms arises through the scattering of the Rydberg electron from an intruding perturber atom. This peculiar interaction gives rise to a plenitude of previously unobserved effects. Within the framework of the present thesis, this interaction is studied in detail for Rydberg
P-states in rubidium. Due to their long lifetime, atoms in Rydberg states are subject to scattering with the surrounding ground state atoms in the ultracold cloud. By measuring their lifetime as a function of the ground state atom flux, we are able to obtain the total inelastic scattering cross section as well as the partial cross section for associative ionisation. The fact that the latter is three orders of magnitude larger than the size of the formed molecular ion indicates the presence of an efficient mass transport mechanism that is mediated by the Rydberg–ground state interaction. The immense acceleration of the collisional process shows a close analogy to a catalytic process. The increase of the scattering cross section renders associative ionisation an important process that has to be considered for experiments in dense ultracold systems. The interaction of the Rydberg atom with a ground state perturber gives rise to a highly oscillatory potential that supports molecular bound states. These so-called ultralong-range Rydberg molecules are studied with high resolution time-of-flight spectroscopy, where we are able to determine the binding energies and lifetimes of the molecular states between the two fine structure split
25P-states. Inside an electric field, we observe a broadening of the molecular lines that indicates the presence of a permanent electric dipole moment, induced by the mixing with high angular momentum states. Due to the mixing of the ground state atom’s hyperfine states by the molecular interaction, we are able to observe a spin-flip of the perturber upon creation of a Rydberg molecule. Furthermore, an incidental near-degeneracy in the underlying level scheme of the
25P-state gives rise to highly entangled states between the Rydberg fine structure state and the perturber’s hyperfine structure. These mechanisms can be used to manipulate the quantum state of a remote particle over distances that exceed by far the typical contact interaction range. Apart from the ultralong-range Rydberg molecules that predominantly consist of only one low angular momentum state, a class of Rydberg molecules is predicted to exist that strongly mixes the high angular momentum states of the degenerate hydrogenic manifolds. These states, the so-called trilobite- and butterfly Rydberg molecules, show very peculiar properties that cannot be observed for conventional molecules. Here we present the first experimental observation of butterfly Rydberg molecules. In addition to an extensive spectroscopy that reveals the binding energy, we are also able to observe the rotational structure of these exotic molecules. The arising pendular states inside an electric field allow us, in comparison to the model of a dipolar rotor, to extract the precise bond length and dipole moment of the molecule. With the information obtained in the present study, it is possible to photoassociate butterfly molecules with a selectable bond length, vibrational state, rotational state, and orientation inside an electric field. By shedding light on various previously unrevealed aspects, the experiments presented in this thesis significantly deepen our knowledge on the Rydberg–ground state interaction and the peculiar effects arising from it. The obtained spectroscopic information on Rydberg molecules and the changed reaction dynamics for molecular ion creation will surely provide valuable data for quantum chemical simulations and provide necessary data to plan future experiments. Beyond that, our study reveals that the hyperfine interaction in Rydberg molecules and the peculiar properties of butterfly states provide very promising new ways to alter the short- and long-range interactions in ultracold many-body systems. In this sense the investigated Rydberg–ground state interaction not only lies right at the interface between quantum chemistry, quantum many-body systems, and Rydberg physics, but also creates many new and fascinating possibilities by combining these fields.
Abstract Understanding Coulomb driven many-body dynamics in ultracold atomic systems far from equilibrium remains an open challenge, particularly when ultrafast excitation channels create competing pathways toward Rydberg gases or ultracold plasmas. Here, we investigate the many-body dynamics in a 87 Rb Bose-Einstein condensate after exposure to a single femtosecond laser pulse. By tuning the laser wavelength across the two-photon ionization threshold, we can control the initial state that is either dominated by free electrons and leads to an ultracold plasma or dominated by electrons in excited states which leads to a dense Rydberg gas. The large bandwidth enables overcoming the Rydberg blockade that limits the excitation density for narrow-linewidth lasers. We directly measure the kinetic energy of the released electrons and compare the final distribution of free, bound and plasma electrons to molecular dynamics simulations where the electrons are modeled as individual particles including collisional ionization and recombination processes. We find very good agreement between the simulated electron distribution and the experimental observation. We identify charge imbalance as main driver for the decay of a dense Rydberg gas into an ultracold plasma.