In this work I describe the excitation spectra of Rydberg atoms in ultracold gases of strontium and their decay mechanisms. In a few-body regime, we observe a highly structured spectrum re ecting excitation of ultralong-range molecules consisting of one or more ground-state atoms bound to the Rydberg core in potential wells formed by the Rydbergelectron wave function. In a many-body regime, with hundreds of ground-state atoms within the Rydberg orbital, the Rydberg atoms can be viewed as an impurity in a quantum gas, connecting to important concepts in condensed matter physics. The spectrum for impurity excitation displays signatures of polaronic states, in which the Rydberg atom signi cantly perturbs the density of the background gas. Additionally, decay channels of Rydberg excitations are examined by monitoring the time evolution of Rydberg populations. The measured lifetimes reveal new information on the decay processes of Rydberg molecules and place 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.
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.
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.
Collisions involving Rydberg atoms reveal detailed information on the state of a background medium and can be used as diagnostic probes of temperature and density distributions in a neutral or ionized gas. Spectroscopy of Rydberg atoms in highly excited states reveals the interaction of the Rydberg electron with core electrons, including relativistic effects, and can be used for precise determination of fundamental constants. The advent of ultracold trapping and cooling methods in the last three decades has ushered in a new paradigm in Rydberg physics control and manipulation. The concept of the Rydberg blockade, for instance, al- lows for precise control of long-range dipolar interaction between atoms, creation of correlated many-body wave functions, and realization of macroscopic quantum entanglement and quan- tum logic operations. The formation of a new class of Rydberg molecules arising from ground and Rydberg atom collisions can be used to manipulate electron-atom scattering phase shifts, form and manipulate molecules with enormous permanent electric dipole moments, study Ry- dberg chemistry at the ultracold, and realize macroscopic quantum polaronic systems. In this thesis, I will investigate charge transfer from covalent ground-Rydberg collisions to form heavy ion pair states. In another related study, I explore the formation of spin-mixed ultralong range Rydberg molecules, by accounting for spin-dependent relativistic fine and hyperfine interac- tion. Such studies help to not only explain experimental observations, but also point to how molecular reactions can be controlled using small electric or magnetic fields.
We report spectroscopic observation of Rydberg polarons in an atomic Bose gas. Polarons are created by excitation of Rydberg atoms as impurities in a strontium Bose-Einstein condensate. They are distinguished from previously studied polarons by macroscopic occupation of bound molecular states that arise from scattering of the weakly bound Rydberg electron from ground-state atoms. The absence of a p-wave resonance in the low-energy electron-atom scattering in Sr introduces a universal behavior in the Rydberg spectral line shape and in scaling of the spectral width (narrowing) with the Rydberg principal quantum number, n. Spectral features are described with a functional determinant approach (FDA) that solves an extended Fröhlich Hamiltonian for a mobile impurity in a Bose gas. Excited states of polyatomic Rydberg molecules (trimers, tetrameters, and pentamers) are experimentally resolved and accurately reproduced with a FDA.
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.