The growth and characterization of room temperature ferromagnetic wideband-gap materials for spintronic applications

Wide-bandgap dilute magnetic semiconductors (DMS), such as transition-metal doped ZnO and GaN, have gained attention for use in spintronic devices because of predictions and experimental reports of room temperature ferromagnetism which may enable their use in spintronic devices. However, there has been some debate over the source of ferromagnetism in these materials. This paper focuses on the high quality growth of wide bandgap DMS, and the characterization of Zn1-xMnxO produced by melt-growth techniques and Ga1-xMnxN grown by metal organic chemical vapor deposition (MOCVD). High resolution X-ray diffraction results revealed no second phases in either the ZnO crystals or the GaN films. Undoped as-grown, bulk crystals of Zn1-xMnxO and Zn1-xCoxO crystals are shown to be paramagnetic at all temperatures. In contrast, the Ga1-xMnxN films showed ferromagnetic behavior at room temperature under optimum growth conditions. Experimental identification of the Mn ion charge state and the presence of bands in the bandgap of GaN are investigated by optical spectroscopy and electron spin paramagnetic resonance (EPR). It is shown that the broadening of states in the Mn 3d shell scaled with Mn concentration, and that optical transitions due to this band correlated with the strong ferromagnetism in these samples. However, this band disappeared with an increase in free electron concentration provided by either annealing or doping. Raman studies of Ga1-xMnxN revealed two predominant Mn-related modes featured with increasing concentration, a broad disorder related structure at 300cm(-1) and a sharper peak at 669cm(-1) This works show that the development of practical ferromagnetic wide bandgap DMS materials for spintronic applications will require both the lattice site introduction of Mn as well as careful control of the background defect concentration to optimize these materials.