Abstract We develop a formalism for photoionization (PI) and potential energy curves (PECs) of Rydberg atoms in ponderomotive optical lattices and apply it to examples covering several regimes of the optical-lattice depth. The effect of lattice-induced PI on Rydberg-atom lifetime ranges from noticeable to highly dominant when compared with natural decay. The PI behavior is governed by the generally rapid decrease of the PI cross sections as a function of angular-momentum (ℓ), lattice-induced ℓ-mixing across the optical-lattice PECs, and interference of PI transition amplitudes from the lattice-mixed into free-electron states. In GHz-deep lattices, ℓ-mixing leads to a rich PEC structure, and the significant low-ℓ PI cross sections are distributed over many lattice-mixed Rydberg states. In lattices less than several tens-of-MHz deep, atoms on low-ℓ PECs are essentially ℓ-mixing-free and maintain large PI rates, while atoms on high-ℓ PECs trend towards being PI-free. Characterization of PI in GHz-deep Rydberg-atom lattices may be beneficial for optical control and quantum-state manipulation of Rydberg atoms, while data on PI in shallower lattices are potentially useful in high-precision spectroscopy and quantum-computing applications of lattice-confined Rydberg atoms.
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 5
D3/2-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.