The Enriched Xenon Observatory (EXO) is a series of experiments seeking to measure the neutrino mass through observation of neutrinoless double beta decay (0nbb). The next generation of 0nbb experiments aims to probe Majorana neutrino masses at or below 10 meV. To reach this sensitivity, ton-scale detectors are needed with lower radioactive backgrounds than the best ones operating today. The EXO collaboration is developing a novel strategy for a virtually background-free search for the 0nbb of Xe-136, based around detecting individual Ba-136 ions resulting from such decays. This dissertation details the efforts to develop a barium tagging technique which uses resonance ionization spectroscopy (RIS) to selectively and efficiently ionize barium atoms for injection and detection in an ion trap. A simple radionuclide-driven single-ion source has been developed to push the technology to high efficiency with a small number of ions.