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Deposition of thin film dielectrics, and in particular for chemical vapor deposition of nano-layer structures comprising multiple layers of dielectrics, such as, silicon dioxide, silicon nitride, silicon oxynitride, and/or other silicon compatible dielectrics includes post-deposition surface treatment of deposited layers with a metal or semiconductor source gas, e.g., a silicon source gas. Deposition of silicon containing dielectrics comprises silane-based chemistry for deposition of doped or undoped dielectric layers, and surface treatment of deposited dielectric layers with silane. Surface treatment provides dielectric layers with improved layer-to-layer uniformity and lateral continuity, and substantially atomically flat dielectric layers suitable for multilayer structures for electroluminescent light emitting structures, e.g., active layers containing rare earth containing luminescent centers. Doped or undoped dielectric thin films or nano-layer dielectric structures may also be provided for other semiconductor devices.