Room-Temperature Ferromagnetism of Cu-Doped ZnO Films Probed by Soft X-Ray Magnetic Circular Dichroism

We report direct evidence of room-temperature ferromagnetic ordering in O-deficient ZnO:Cu films by using soft x-ray magnetic circular dichroism and x-ray absorption. Our measurements have revealed unambiguously two distinct features of Cu atoms associated with (i) magnetically ordered Cu ions present only in the oxygen-deficient samples and (ii) magnetically disordered regular Cu2+ ions present in all the samples. We find that a sufficient amount of both oxygen vacancies (V-O) and Cu impurities is essential to the observed ferromagnetism, and a non-negligible portion of Cu impurities is uninvolved in the magnetic order. Based on first-principles calculations, we propose a microscopic indirect double-exchange model, in which alignments of localized large moments of Cu in the vicinity of the VO are mediated by the large-sized vacancy orbitals.