Copper (Cu) thin films have been widely used as electrodes and interconnection wires in integrated electronic circuits, and more recently as substrates for the synthesis of graphene. However, the ultra-high vacuum processes required for high-quality Cu film fabrication, such as molecular beam epitaxy (MBE), restricts mass production with low cost. In this work, we demonstrated high-quality Cu thin films using a single-crystal Cu target and radio-frequency (RF) sputtering technique; the resulting film quality was comparable to that produced using MBE, even under unfavorable conditions for pure Cu film growth. The Cu thin film was epitaxially grown on an Al2O3 (sapphire) (0001) substrate, and had high crystalline orientation along the (111) direction. Despite the 10−3 Pa vacuum conditions, the resulting thin film was oxygen free due to the high chemical stability of the sputtered specimen from a single-crystal target; moreover, the deposited film had >5× higher adhesion force than that produced using a polycrystalline target. This fabrication method enabled Cu films to be obtained using a simple, manufacturing-friendly process on a large-area substrate, making our findings relevant for industrial applications.

Oxygen vacancy (VO) strongly affects the properties of oxides. In this study, we used X-ray diffraction (XRD) to study changes in the VO concentration as a function of the Co-doping level of ZnO. Rietveld refinement yielded a different result from that determined via X-ray photoelectron spectroscopy (XPS), but additional maximum entropy method (MEM) analysis led it to compensate for the difference. VO tended to gradually decrease with increased Co doping, and ferromagnetic behavior was not observed regardless of the Co-doping concentration. MEM analysis demonstrated that reliable information related to the defects in the ZnO-based system can be obtained using X-ray diffraction alone.

We investigated the effects of Al doping on ferromagnetism in Co-doped ZnO and the mechanisms that give rise to ferromagnetism in hydrogen-injected ZnCoO. The aim of this study was to determine whether the occurrence of ferromagnetism or the strength of the magnetization is related to the charge carrier mobility, charge carrier density, or the presence of defects in the crystal lattice. Al doping increased the carrier density, as well as the density of oxygen vacancies and the lattice strain; however, these physical properties were not related to the changes in magnetism. Al-doped and undoped ZnCoO showed an increase in ferromagnetism as a function of the hydrogen plasma treatment time. Al doping suppressed the hydrogen-mediated ferromagnetism in ZnCoO:H by trapping hydrogen via oxygen vacancies created by Al doping.

Hydrogen-treated ZnCoO shows magnetic behavior, which is related to the formation of Co-H-Co complexes. However, it is not well known how the complexes are connected to each other and with what directional behavior they are ordered. In this point of view, ZnCoO nanowire is an ideal system for the study of the magnetic anisotropy. ZnCoO nanowire was fabricated by trioctylamine solution method under different ambient gases. We found that the oxidation of trioctylamine plays an essential role on the synthesis of high-quality ZnCoO nanowires. The hydrogen injection to ZnCoO nanowires induced ferromagnetism with larger magnetization than ZnCoO powders, while becoming paramagnetic after vacuum heat treatment. Strong ferromagnetism of nanowires can be explained by the percolation of Co-H-Co complexes along the c-axis.

Manipulation of spin ordering in oxides without extrinsic contribution is an important issue in current spintronics. This study introduced a mechanism to ascertain the formation of magnetic clusters and the magnetism of a Co-doped ZnO system by temperature-dependent magnetic susceptibility measurements. The measurements demonstrate the possibility of detecting tiny portions of Co clusters that could be created from Co oxides that were undetectable in X-ray diffraction or transmission electron microscopy. By fitting the magnetic susceptibility results, we were also able to ascertain that pure Co-doped ZnO showed a negative Curie-Weiss temperature, implying the existence of antiferromagnetic ordering; however, the Curie-Weiss temperature was gradually increased by intentional hydrogen introduction, with results suggesting that the antiferromagnetic ordering declined proportionally to the hydrogen contents by hydrogen mediation in Co-Co spin ordering and induced ferromagnetism. These results provide a useful methodological approach as well as experimental clues for identifying the origin of magnetism.