Defect-Driven Magnetism in Luminescent n/p-Type Pristine and Gd-Substituted SnO₂ Nanocrystalline Thin Films

The effects of rare-earth-element Gd doping on the intrinsic magnetic ordering, photoluminescence, and electrical-conducting properties of the pristine SnO(2) nanocrystalline thin films fabricated by radio-frequency (RF) sputtering are investigated. The pristine SnO(2) thin film exhibits significant ferromagnetism while Gd doping results in an absence of intrinsic ferromagnetism. The presence of large amounts of singly ionized oxygen vacancies (V(O)(+)) is traced by photoluminescence spectroscopic analysis and they are found to be responsible for the observed ferromagnetism in pristine SnO(2) thin films. A significant reduction of oxygen vacancies is observed after Gd doping, and that might be insufficient to mediate long-range ferromagnetic ordering between V(O)(+) defects in a Gd-doped SnO(2) system. Although the associated magnetic moment is increased by 1 order of magnitude, because of the insertion of Gd(3+) ions, which have localized f-shell paramagnetic moment, there is no intrinsic FM ordering. Hall measurement reveals that the pure SnO(2) exhibits n-type behavior whereas Gd-doped SnO(2) films show the p-type conductivity with higher resistivity. The studies demonstrate that only structural defects such as V(O)(+) defects, not magnetic ions such as Gd(3+), are responsible for inducing ferromagnetism in SnO(2) thin films.