In this thesis, we examine the ponderomotive interaction between an applied optical field and a highly excited Rydberg electron. An atom in a Rydberg state is essentially composed of an electron loosely bound, at a relatively large radial separation, to a positive ionic core. As such, the ponderomotive interaction for the Rydberg electron is similar to the interaction with free charges, which has been studied in context of plasma physics, new particle accelerator techniques, ion trapping, and electron diffraction among others. We are focused on using the ponderomotive interaction with the Rydberg electron to exert control over both the center-of-mass and electronic states of translationally cold Rydberg atoms. These capabilities can be adapted as tools for application in many experiments in areas such as atomic spectroscopy and quantum information processing. Our theoretical investigations have provided a well-defined parameter space for our experimental work and have allowed us to develop experimental methods appropriate for studying Rydberg atoms in ponderomotive potentials. In dense gases of cold Rydberg atoms, rich dynamics stem from electric multipole interactions among the Rydberg atoms. For example, interatomic forces between Rydberg atoms cause state-changing collisions which can significantly increase the kinetic energy of the colliding atoms. In addition to the studies of Rydberg atoms in ponderomotive potentials, we discuss collisions of cold Rydberg atoms in which internal energy of the Rydberg atoms is converted into kinetic energy.
In this thesis, we examine the ponderomotive interaction between an applied optical field and a highly excited Rydberg electron. An atom in a Rydberg state is essentially composed of an electron loosely bound, at a relatively large radial separation, to a positive ionic core. As such, the ponderomotive interaction for the Rydberg electron is similar to the interaction with free charges, which has been studied in context of plasma physics, new particle accelerator techniques, ion trapping, and electron diffraction among others. We are focused on using the ponderomotive interaction with the Rydberg electron to exert control over both the center-of-mass and electronic states of translationally cold Rydberg atoms. These capabilities can be adapted as tools for application in many experiments in areas such as atomic spectroscopy and quantum information processing. Our theoretical investigations have provided a well-defined parameter space for our experimental work and have allowed us to develop experimental methods appropriate for studying Rydberg atoms in ponderomotive potentials. In dense gases of cold Rydberg atoms, rich dynamics stem from electric multipole interactions among the Rydberg atoms. For example, interatomic forces between Rydberg atoms cause state-changing collisions which can significantly increase the kinetic energy of the colliding atoms. In addition to the studies of Rydberg atoms in ponderomotive potentials, we discuss collisions of cold Rydberg atoms in which internal energy of the Rydberg atoms is converted into kinetic energy.
In this dissertation, I explore several aspects of Rydberg physics with laser spectroscopy. The experiments center around the use of a very deep, cavity-generated, one-dimensional optical lattice in a cold atom sample. The optical lattice produces elongated clouds of dense, cold atoms via dipole trapping and is able to generate extreme light shifts in the atoms due to its high intensity. I describe experiments which may be divided into two main classes. In the first, I use the dipole trap to prepare a dense sample of atoms for photoassociation of Rb atom pairs into diatomic Rydberg molecules. The Rydberg molecules are formed by low-energy scattering of the Rydberg electron of one atom from the other atom, which is a ground-state atom. This novel binding mechanism also has relevance for chemical physics. I present binding energy measurements for eight different cases of Rydberg molecules. The binding energies reveal information about electron-atom collisions, such as their scattering lengths, and about the spin couplings present within the molecular system. In the second class of experiments, I introduce two proposed measurements in which the optical lattice is ramped to very high intensity during the laser excitation, creating AC Stark shifts in the transition frequencies. In one measurement, low-lying atomic states are probed. Measurements of the light shifts are expected to yield data on the dynamic polarizability and the photoionization cross section of the 5D3/2-state in rubidium in a 1064-nm light field. I show corresponding preliminary experimental data. The polarizability and photo-ionization cross-section measurements will provide tests of atomic structure theory, which is important both at a fundamental level and for applications such as atomic clocks. In another proposed measurement, Rydberg atoms in the lattice experience ponderomotive shifts and strong mixing of their angular-momentum states, allowing direct optical excitation of the lattice-mixed high-angular-momentum states. I describe the theoretical basis and experimental preparation for spectroscopically characterizing the lattice-mixed states. The ability to optically excite selected high-angular-momentum states without the use of static or RF fields may be useful for quantum information processing and simulation.
Using cold atoms, I probe the energy-level intervals between Rydberg states to high spectroscopic precision. The focus of this work is to lay the groundwork for an updated, highly-controlled measurement of the Rydberg constant using circular-state Rydberg atoms, needed to resolve a recent conflict in proton-radius values that arose in 2010 (the so-called 'proton radius puzzle'). Toward this end, I have demonstrated a fundamentally-new mechanism with which to drive atomic (Rydberg-Rydberg) transitions, utilizing an inelastic (state-changing) ponderomotive interaction. Until now, the multipole-field interaction has been the sole mechanism on which spectroscopy of atomic transitions has been based. In this work, the state-changing ponderomotive interaction ('ponderomotive spectroscopy') is demonstrated by amplitude-modulating an optical standing wave at a transition resonance of a Rydberg atom. At the core of this new spectroscopic technique is the requirement that the light intensity must be modulated in space within the atomic volume, and in time at the desired atomic transition frequency. A Rydberg atom in a modulated optical lattice is very well-suited for a demonstration of this novel type of spectroscopy. Magic-wavelength conditions of this interaction are also identified, as well as a method to drive transitions at harmonics of the modulation. Both of these features of ponderomotive spectroscopy will be utilized to simultaneously trap and probe Rydberg atoms to perform the Rydberg constant measurement. I also present a high-precision measurement of the quantum defect of a high-angular-momentum state of rubidium, the atomic species that will be used in the Rydberg constant measurement. The quantum defects of high-angular-momentum states are needed to determine the effect of the rubidium core polarizability on the Rydberg constant measurement, which is anticipated to be a leading uncertainty. Finally, I present the background and design work for a measurement of the Rydberg constant specifically tailored to help resolve the proton radius puzzle, thereby completing the major preliminary work needed for the performance of that high-precision measurement.
I examine the trapping of Rydberg atoms in an optical standing wave. This trap, called an optical lattice, offers a platform for utilizing Rydberg atoms and their unique properties in applications such as atomic spectroscopy and quantum computing. Toward this end, I demonstrate the capability to trap rubidium 85 Rydberg atoms in a one-dimensional 1064 nm wavelength optical lattice with high efficiency. I have achieved a 90% trapping efficiency by inverting the lattice immediately after Rydberg-atom excitation, using an electro-optic technique. In addition, I investigate the dependence of optical-lattice trapping potentials for Rydberg atoms on the angular portion of the atomic wavefunction. While ground-state atoms are point-like in relation to an optical-lattice field, Rydberg-atom wavefunctions extend over a substantial fraction of the lattice period, leading to an angular dependence of the lattice trapping potentials. I measure the potentials using various angular sublevels of Rydberg nD states prepared in the optical lattice with a superimposed transverse DC electric field. This unique angular dependence of Rydberg-atom optical lattices may be exploited to tailor the trapping potentials as needed for spectroscopy or quantum computing. Further, atom loss due to lattice-induced photoionization of Rydberg atoms must be characterized for applications. I investigate the photoionization process as a function of position within the volume of a Rydberg atom. Since Rydberg-atom sizes approximately equal the lattice period, the lattice intensity varies maximally within the atomic volume. I find that photoionization rates are higher for lattice intensity maxima located near the nucleus than within the lobes of the electronic probability distribution. Photoionization therefore occurs near the Rydberg-atom nucleus. Finally, I calculate photoionization rates for Rydberg atoms in optical fields and investigate how these rates relate to the validity of the electric dipole approximation. This approximation is usually central to matter-field interactions, and Rydberg atoms in optical fields present a system for studying the approximation in a limiting case. I further apply the photoionization calculations to experimentally-relevant conditions. With these advances, this thesis lays essential groundwork for the employment of Rydberg-atom optical lattices in applications.
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.
We have studied the development of gases of ultra-cold Rydberg atoms in Magneto Optic Traps, and discovered that such gases exhibit a range of density-dependent phenomena. In particular, we have found that at the densities of ∼ 10 7 cm -3 the Rydberg atoms spontaneously evolve into long-lived high angular momentum states. These states slowly decay due to microwave background radiation over tens of milliseconds. We have numerically simulated the effects leading to such behavior, and investigated numerically the l- and n-mixing collisions of Rydberg atoms with electrons in the range of 10 meV. These calculations show that the l- and n-mixing cross-sections follow the n 5 scaling law, expected from simple Stark map considerations, but also depend on the velocities of the colliding electrons, reflecting the adiabaticity of the atom-electron interactions. We have developed a novel technique of measuring the electric fields inside plasmas by using Rydberg excitation spectroscopy of embedded atoms, based on the disappearance of regions of zero oscillator strength in the presence of such fields. We have applied this technique to study the evolution of ultra-cold non-neutral plasmas excited from the MOT, and have found that it expands over 1 mus. We have simulated such an expansion by considering only Coulomb repulsion between the constituent ions, and have found that such a model is consistent with the experimental observations.
We have observed the evolution of cold Rydberg gases and ultracold plasmas in an environment that allows for the control of interactions of the blackbody radiation temperature from 4K to 300K. The work in this thesis describes the influence of initial densities, populations, excitation state, evolution time and thermal background temperature on the evolution of cold Rydberg gases as well as directly excited ultracold plasmas. With some initial ionization, cold-Rydberg-atom gases easily develop a positive space charge that traps electrons for times on the order of tens of mus. This acts as a catalyst for electron-Rydberg atom collisions, increasing the collision probabilities by orders of magnitude and profoundly altering the final state of the Rydberg gas. Using state-selective field ionization, we have provided direct proof that these collisions cause changes in l-states, and we have seen the first experimental evidence that they also lead to inelastic n-changing collisions, as predicted by theory. We have also found evidence for Rydberg-Rydberg collisions, enabled by the attractive electric-dipole forces between atoms in high-l states and possibly by van-der-Waal's interactions at very high-n . Thermal interactions are seen to influence the formation of a plasma from a cold Rydberg gas. Plasmas form more easily in the presence of a 300K radiation field than at 4K, due to the contribution of thermal ionization to the plasma formation. The background temperature also appears to affect the electron temperature in both the directly excited plasma and the plasma spontaneously formed from a cold Rydberg gas. In Rydberg atom gases that have undergone partial ionization, electron temperatures were estimated using the dependence of n-changing collisions on the electron temperature.