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The surface Cs–O activation process directly determines quantum efficiency and stability of negative-electron-affinity photocathodes. To investigate the effects of excessive Cs and O supply on activation and to explore a more effective Cs–O activation recipe, Cs–O activation experiments of GaAs(100) photocathodes are carried out based on the current-driven solid Cs and O dispensers. By a comparison of differences in activation photocurrent, quantum efficiency, and photocurrent decay, it is found that the recipe of excessive O and non-excessive Cs is not suitable for activating GaAs photocathodes, while the recipe of continuous and completely excessive Cs along with intermittent and non-excessive O can achieve the most excellent photoemission performance, including the highest quantum efficiency in the long-wave threshold region and best stability under intense light irradiation after activation. Furthermore, this improved activation recipe with the least Cs–O alternating cycles is easier to operate. Combined with density functional calculations and dipole layer model, it is found that the activation recipe of completely excessive Cs and non-excessive O can form effective dipoles to the greatest extent, and avoid the direct interaction between As atoms and O atoms to form As–O–Ga oxides on the GaAs(100) reconstructed surface.

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