Thesis (Ph. D.)--University of Washington, 2003This thesis describes the development and implementation of a new scheme for observing RF transitions between spin states in a single, trapped Ba + ion. We use optical pumping to place the ion in a selected magnetic sublevel of either the 6S1/2 ground state or the 5D3/2 metastable state. The ion is exposed to an RF field, and a spin-sensitive version of the electron shelving method detects the resulting spin state. The precision of this kind of RF spectroscopy is limited only by magnetic-field noise, and with the current apparatus, line widths of about 10 Hz can be achieved.This scheme is applied to a precision measurement of light shifts (or AC Stark shifts) in Ba+. Zeeman energies are altered...