Embodiments of the invention provide methods for forming a dielectric stack by exposing a substrate to a sequence of deposition, nitridation and annealing processes. In one example, a method includes exposing the substrate to a deposition process to form a dielectric layer thereon, exposing the substrate to a nitridation process to form a nitride layer thereon, exposing the substrate to an annealing process and exposing the substrate sequentially to the deposition and nitridation processes while periodically and intermediately exposing the substrate to the annealing process to form a dielectric material having a predetermined thickness. Generally, a nitrogen plasma is used during the nitridation process to form a nitrogen concentration within a range from about 5 atomic percent (at%) to about 25 at%. The dielectric layers usually contain oxygen and at least one additional element, such as hafnium, tantalum, titanium, aluminum, zirconium, lanthanum, silicon or combinations thereof. |