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Electronic correlation in anion p orbitals impedes ferromagnetism due to cation vacancies in Zn chalcogenides.

Electronic correlation effects, usually associated with open d or f shells, have so far been considered in p orbitals only sporadically for the localized 2p states of first-row elements. We demonstrate that the partial band occupation and the metallic band-structure character as predicted by local density calculations for II-VI materials containing cation vacancies is removed when the correct energy splitting between occupied and unoccupied p orbitals is recovered. This transition into a Mott-insulating phase dramatically changes the structural, electronic and magnetic properties along the entire series (ZnO, ZnS, ZnSe, and ZnTe), and impedes ferromagnetism. Thus, important correlation effects due to open p shells exist not only for first-row (2p) elements, but also for much heavier anions like Te (5p).