A method is provided for forming a nitrided high-k film in an atomic layer deposition process (ALD) process. The method includes receiving a substrate in a process chamber, maintaining the substrate at a temperature sufficient for ALD of a nitrided high-k film, and depositing the nitrided high-k film on the substrate by exposing the substrate to a gas pulse sequence that includes, in any order: a) exposing the substrate to a gas pulse comprising a metal-containing precursor, b) exposing the substrate to a gas pulse comprising an oxygen-containing gas, and c) exposing the substrate to a gas pulse comprising trisilylamine gas, where the exposing the substrate to the trisilylamine gas yields the nitrided high-k film that includes nitrogen and that is substantially free of silicon, and repeating the gas pulse sequence. A trisilylamine gas exposure may also be used to nitride a deposited high-k film.