Embodiments of the invention provide methods for forming silicon oxynitride materials on a substrate. In one embodiment, a method for forming a dielectric material on a substrate is provided which includes positioning a substrate containing a native oxide surface within a processing system containing a plurality of process chambers, and removing the native oxide surface to form a substrate surface free of native oxide during a clean process. The method further provides exposing the substrate to a first nitrogen-containing plasma to form a silicon nitride layer from the substrate surface during a first nitridation process, exposing the substrate to an oxygen source to form a silicon oxynitride layer from the silicon nitride layer during a thermal oxidation process, exposing the substrate to a second nitrogen-containing plasma during a second nitridation process, and exposing the substrate to an annealing process.