We have investigated ternary metal oxide films for high-k gate dielectrics by using a layer-by-layer deposition & annealing method so as to keep the dielectric constant of the film high with no crystallization. HfAlOx films have been prepared by alternating deposition of HfO2 and Al2O3 layers, where it is a key for the improvement of the film quality to understand the intermixing process between two layers by thermal treatments. So, we first discuss the atomic diffusion and structural change of the HfO2/Al2O3 “superlattice” film as a function of the annealing temperature by changing the Hf/Al ratio. In a typical case of the film with HfOx/AlOx=3Å/9Å cycle, a clear superlattice peak is observed below 750 °C by XRD. Above 850 °C, a different type of crystalline structure with no superlattice peaks is observed. These results indicate that the intermixing in HfO2/Al2O3 (3Å/9Å) films occurs between 750 and 850 °C. The intermixing onset temperature increases with increasing Al content in Hf/Al ratio.
To further increase the crystallization temperature, nitrogen incorporation into the film is considered, and effects of the nitrogen incorporation into HfAlOx films are studied from the structural and electrical viewpoints. The results indicate that there is a tradeoff between crystallization restriction and leakage current degradation for the nitrogen incorporation into HfAlOx films.