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Spectroscopic and atom-optics experiments on Rydberg He in electric and magnetic fields: towards low-temperature investigations of ion-molecule chemistry involving He+

Matija Žeško

Published Jan 1, 2019• 0 citations
Publisher
DOI
10.3929/ethz-b-000366310

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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.
Laser cooling of atomic ions has long been used as a tool in physics to explore quantum entanglement for applications in quantum computing and information. More recently, laser-cooled atomic ions have been used as a platform for studying cold chemistry. Here, we describe an experimental system called a “Coulomb crystal,” where laser-cooled ions are confined in traps at sufficiently low translational energies that they form an ordered structure. We then present a range of experiments undertaken using this platform, from studies of reactions with an atomic species to reaction systems of increased complexity, involving molecular ions and neutral molecules. We also describe a few spectroscopic studies enabled by Coulomb crystals before discussing some possible future directions of the field. This is not meant to be a comprehensive review of the entire field, but rather a sampling of the types of experiments that can be performed and the knowledge gained from these studies.
Rydberg molecule, formed by one or more Rydberg atoms, exhibits remarkable properties, including an exceptionally large spatial extent, rich rovibrational level structures, permanent electric dipole moments, and a pronounced sensitivity to external fields. Based on the underlying binding mechanisms, Rydberg molecules can be divided into three categories, the ground-Rydberg molecule that is bound via a low-energy electron-atom scattering interaction between ground atom and Rydberg electron, the Rydberg-Rydberg molecule that is bound via a long-range electrostatic interaction between Rydberg atoms, and the ion-Rydberg molecule that is bound via single- or multi-polar interactions between Rydberg atom and ion. This review focuses on recent theoretical and experimental advances in diatomic Rydberg molecules, covering their formation and binding mechanisms, potential energy curves, experimental observations, and spectroscopic properties, with the aim of providing a comprehensive overview of the current state and future prospects of this rapidly developing field.