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Halide vacancies and associated metallic lead (Pb°) observed at the surface and deep inside macroscopic organolead trihalide perovskite crystals is removed through a facile and noninvasive treatment. Indeed, Br2 vapor is shown to passivate Br-vacancies and associated Pb° in the bulk of macroscopic crystals. Controlling the exposure time can markedly improve the overall stoichiometry for moderate exposures or introduce excessive bromide for long exposures, resulting in p-doping of the crystals. In the low dose passivation regime, Hall ef