High quantum efficiency, robust photocathodes produce picosecond-pulsed, high-current electron beams for photoinjection applications like free electron lasers. In photoinjectors, a pulsed drive laser incident on the photocathode causes photoemission of short, dense bunches of electrons, which are then accelerated into a relativistic, high quality beam. Future free electron lasers demand reliable photocathodes with long-lived quantum efficiency at suitable drive laser wavelengths to maintain high current density. But faced with contamination, heating, and ion back-bombardment, the highest efficiency photocathodes find their delicate cesium-based coatings inexorably lost. In answer, the work herein presents careful, focused studies on cesium-based photocathodes, particularly motivated by the cesium dispenser photocathode. This is a novel device comprised of an efficiently photoemissive, cesium-based coating deposited onto a porous sintered tungsten substrate, beneath which is a reservoir of elemental cesium. Under controlled heating cesium diffuses from the reservoir through the porous substrate and across the surface to replace cesium lost to harsh conditions -- recently shown to significantly extend the lifetime of cesium-coated metal cathodes. This work first reports experiments on coated metals to validate and refine an advanced theory of photoemission already finding application in beam simulation codes. Second, it describes a new theory of photoemission from much higher quantum efficiency cesium-based semiconductors and verifies its predictions with independent experiment. Third, it investigates causes of cesium loss from both coated metal and semiconductor photocathodes and reports remarkable rejuvenation of full quantum efficiency for contaminated cesium-coated surfaces, affirming the dispenser prescription of cesium resupply. And fourth, it details continued advances in cesium dispenser design with much-improved operating characteristics: lower temperature and cleaner operation. Motivated by dispenser integration with semiconductor coatings, initial fabrication of those coatings are reported on dispenser-type substrates with measurement of quantum efficiency and analysis of thermal stability. Detailed investigations are performed on dispenser substrate preparation by ion beam cleaning and on dispenser pore structure by electron microscopy and focused ion beam milling. The dissertation concludes by discussing implications of all results for the demonstration and optimization of the future high quantum efficiency cesium dispenser photocathode.