Magnetism driven by non-metal interstitials from first-principles prediction: The case of hydrogen- and fluorine-doped calcium monoxide with rock-salt structure

Our first-principles calculations based on density functional theory confirmed the formation of sp-ferromagnetic states of calcium monoxide with interstitial nonmagnetic F or H atoms. The hydrogen and fluorine interstitials in the oxides were found to be spin polarized and are more stable in the antiferromagnetic state and the ferromagnetic state, respectively. For H-doped CaO, no considerable charge transfer takes place and the spin remains localized on the impurity. For F-doped oxide, the observation may be attributed to the p–p interaction and the charge transfer between the interstitial atom and the neighboring O atoms. We demonstrate that H-doped compound is a potential n-type antiferromagnet, while F-doped material is a potential p-type ferromagnet. The different dopants would induce different magnetic couplings, thus show different ground-state magnetic configurations. The mechanism for the magnetism should be useful for understanding d0 magnetic semiconductors or insulators. The present potential d0 diluted magnetic materials, at least some of them, may be useful in spintronics.