Structural imperfections and attendant localized/itinerant ferromagnetism in ZnO nanoparticles

Abstract

Using synchrotron-based x-ray magnetic spectroscopy, we report a study focusing on the local symmetry of Cu-dopant and resultant structural imperfections in mediating Cu-doped ZnO nanoparticles\' ferromagnetism (FM). Prepared by an antisolvent method, Cu appeared to preferably populate on the basal plane of ZnO with a local symmetry of [CuO4]. This unique symmetry was antiferromagnetic in nature, while electronically and structurally coupled to surrounded oxygen vacancies (V-o) that yielded a localized FM, because of a strong dependency on the number/location of the [CuO4] symmetry. Surprisingly, the FM of undoped but oxygen-deficient ZnO appeared to be more itinerant and long-range, where V-o percolated the FM effectively and isotropically through oxygen\'s delocalized orbital. By adopting the approach of structural imperfection, this study clearly identifies V-o\'s (defect\'s) true characters in mediating the FM of magnetic semiconductors which has been thought of as a long-standing debate, and thus provides a different thinking about the traditional extrinsic ferromagnetic-tuning in the semiconductors. It even illuminates recent research concerning the intrinsic FM of low-dimensional systems that contain defects but non-magnetic elements.