As a two-dimensional material with a hollow hexatomic ring structure, Néel-type anti-ferromagnetic (AFM) GdI3 can be used as a theoretical model to study the effect of electron doping. Based on first-principles calculations, we find that the Fermi surface nesting occurs when more than 1/3 electron per Gd is doped, resulting in the failure to obtain a stable ferromagnetic (FM) state. More interestingly, GdI3 with appropriate Mg/Ca doping (1/6 Mg/Ca per Gd) turns to be half-metallic FM state. This AFM−FM transition results from the transfer of doped electrons to the spatially expanded Gd-5d orbital, which leads to the FM coupling of local half-full Gd-4f electrons through 5d−4f hybridization. Moreover, the shortened Gd−Gd length is the key to the formation of the stable ferromagnetic coupling. Our method provides new insights into obtaining stable FM materials from AFM materials.
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