The evolution of the structural and magnetic properties of Co doped ZnO has been investigated over an unprecedented concentration range above the coalescence limit. ZnO films with Co concentrations from 20% to 60% of the cationic lattice have been grown by reactive magnetron sputtering. The wurtzite crystal structure was maintained even for these high dopant concentrations. By measuring the x-ray absorption at the near edge and the linear and circular dichroism of the films at the Zn and Co K edge, it could be shown that Co substitutes predominantly for Zn in the lattice. No indications of metallic Co have been found in the samples. At low Co concentrations, the films are paramagnetic, but with increasing Co content, the films become antiferromagnetically ordered with increasing order temperature. Uncompensated spins, coupled to the antiferromagnetic dopant configurations, lead to a vertical exchange-bias-like effect, which increases with increasing Co concentration. In parallel, the single-ion anisotropy is gradually lost.

An in-depth analysis of Zn/Al-doped nickel ferrites grown by reactive magnetron sputtering is relevant due to their promising characteristics for applications in spintronics. The material is insulating and ferromagnetic at room temperature with an additional low magnetic damping. By studying the complex interplay between strain and cation distribution their impact on the magnetic properties, i.e., anisotropy, damping, and g-factor is unravelled. In particular, a strong influence of the lattice site occupation of Ni 2+ Td and cation coordination of Fe 2+ Oh on the intrinsic damping is found. Furthermore, the critical role of the incorporation of Zn 2+ and Al 3+ is evidenced by comparison to a sample of altered composition. Specifically, the dopant Zn 2+ is evidenced as a tuning factor for Ni 2+ Td and therefore unquenched orbital moment directly controlling the g-factor. A strain-independent reduction of the magnetic anisotropy and damping by adapting the cation distribution is demonstrated.

Heterostructures of Co-doped ZnO and Permalloy were investigated for their static and dynamic magnetic interaction. The highly Co-doped ZnO is paramagentic at room temperature and becomes an uncompensated antiferromagnet at low temperatures, showing a narrowly opened hysteresis and a vertical exchange bias shift even in the absence of any ferromagnetic layer. At low temperatures in combination with Permalloy an exchange bias is found causing a horizontal as well as vertical shift of the hysteresis of the heterostructure together with an increase in coercive field. Furthermore, an increase in the Gilbert damping parameter at room temperature was found by multifrequency FMR evidencing spin pumping. Temperature dependent FMR shows a maximum in magnetic damping close to the magnetic phase transition. These measurements also evidence the exchange bias interaction of Permalloy and long-range ordered Co-O-Co structures in ZnO, that are barely detectable by SQUID due to the shorter probing times in FMR.

Low temperature Co K-edge x-ray magnetic circular dichroism spectra at different field cooling conditions were recorded to study the imprinted magnetization in antiferromagnetic (AFM) Co doped ZnO (Co:ZnO) films which manifests itself in a vertical exchange bias effect. Co:ZnO films with 50% and 60% doping concentrations were investigated to provide a high degree of pinned magnetic moments. The measurements reveal a change at the main absorption energy of the spectra, while the signal obtained at the pre-edge stays unaffected by the cooling conditions. Therefore, the pinned uncompensated AFM moments, resulting in an imprinted magnetization, are predominantly of orbital character and are independent of ferromagnetic layers.

The structural and magnetic properties of 30% and 50% Co-doped ZnO have been investigated in order to determine the influence of the presence of Co 3+ as a potential p-type dopant. For 30% doping, Co 3+ could be stabilized in the wurtzite lattice of ZnO without phase separation by providing high oxygen partial pressures during growth. At 50% Co concentration, the crystal lattice destabilizes. X-ray absorption spectroscopy and simulations are used to substantiate the valence and local structure of Co 3+ . Integral and element selective magnetometry reveals uncompensated antiferromagnetism of the Co atoms irrespective of being present as Co 2+ or Co 3+ .