Microstructural effect of gadolinium oxide nanocrystals upon annealing on electrical properties of memory devices

The microstructure evolution of sputtered gadolinium oxide nanocrystal (NC) memory devices upon annealing has been characterized in detail by transmission electron microscopy (TEM) and X-ray photoelectron spectroscopy (XPS). TEM results indicate that the as-deposited film is composed of metallic Gd clusters embedded in an amorphous GdxOy matrix. The Gd clusters undergo phase transformation to oxide NCs upon annealing, reaching a maximum density of 7.9–9.1×1011cm−2 at 850°C, which is consistent with the largest memory window width. Upon annealing at even higher temperature, TEM diffraction patterns and XPS composition profiles indicate apparent Si diffusion into the NC layer, probably from the SiO2 tunneling oxide or the Si substrate, leading to the formation of gadolinium silicate NCs. The presence of silicate NCs gradually deteriorates the device performance due to the reduction of barrier confinement for stored charges, although the dot density is only marginally decreased. The results suggest that the optimum memory device performance is dominated by not only the most considered size and density of NCs, but also the composition and phase inside. ► Memory devices with gadolinium oxide nanocrystals have been realized. ► X-ray photoelectron spectroscopy shows annealing-induced interdiffusion of Si. ► Transmission electron microscopy indicates the formation of gadolinium silicate. ► Migrating Si from substrate can further modify NC phase upon annealing. ► Both nanocrystal density and phase influence the device performance.