Embodiments described herein provide a self-limiting and saturating Si—Ox bilayer process which does not require the use of a plasma or catalyst and that does not lead to undesirable substrate oxidation. Methods of the disclosure do not produce SiO2, but instead produce a saturated Si—Ox film with —OH termination to make substrate surfaces highly reactive towards metal ALD precursors to seed high nucleation and growth of gate oxide ALD materials.