The magnetic properties of Gd-doped ZnO films and nanostructures are important to
the development of next-generation spintronic devices. Here, we elucidate the
significant role played by Gd-oxygen-deficiency defects in mediating/inducing
ferromagnetic coupling in in situ Gd-doped ZnO thin films deposited at low oxygen
pressure by pulsed laser deposition (PLD). Samples deposited at higher oxygen
pressures exhibited diamagnetic responses. Vacuum annealing was used on these
diamagnetic samples (grown at a relatively high oxygen pressures) to create oxygen-
deficiency defects with the aim of demonstrating reproducibility of room-temperature
ferromagnetism (RTFM). Samples annealed at oxygen environment exhibited super-
paramagnetism and blocking-temperature effects. The samples possessed secondary
phases; Gd segregation led to superparamagnetism. Theoretical studies showed a shift
of the 4f level of Gd to the conduction band minimum (CBM) in Gd-doped ZnO
nanowires, which led to an overlap with the Fermi level, resulting in strong exchange
coupling and consequently RTFM.
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