Plasma oxidation of thin aluminum layers for magnetic spin-tunnel junctions

This article presents results of a study initiated to characterize the plasma-oxidation process of very thin Al films, a technology commonly used to produce good barrier layers for magnetic spin-tunnel junctions. The behavior of oxygen in the oxidizing Al layer is determined using both quantitative (Rutherford backscattering spectrometry, transmission electron microscopy) and qualitative (x-ray photoelectron spectroscopy (XPS), secondary ion mass spectrometry) analytical techniques. We have applied in situ XPS and experimented with ${}^{18}{\mathrm{O}}_{\mathrm{2}}$ to unravel details of the oxidation mechanism. In addition, the influence of the oxygen pressure on the oxidation rate was established, both with and without a plasma being present. From optical emission spectra it is concluded that this pressure has a minor effect on the relative abundance of excited species in the oxygen plasma. When combined, these data constitute the basis of a model that distinguishes several steps in the plasma oxidation of Al. At the start, oxygen penetrates rapidly throughout the total Al layer, followed by a period of increasing oxygen concentration but constant oxide thickness. Finally, the Co underlayer becomes involved in the oxidation process, which marks the deterioration of the spin-tunnel junction. Evidence is obtained that for the thicker initial Al layers the Co electrode layer starts to oxidize before completion of the Al oxidation. This explains why for 0.8-nm-thick Al films the highest tunnel-magnetoresistance effect is obtained for stoichiometric ${\mathrm{Al}}_{\mathrm{2}}{\mathrm{O}}_{\mathrm{3}},$ whereas for 1.5 nm Al this occurs while the oxide is still substoichiometric.