Role of Trimethylaluminum in Low Temperature Atomic Layer Deposition of Silicon Nitride DangerfieldAaron NanayakkaraCharith E. MallikarjunanAnupama LeiXinjian PearlsteinRonald M. Derecskei-KovacsAgnes CureJeremy EstèveAlain ChabalYves J. 2017 Aminosilanes are attractive precursors for atomic layer deposition of silicon oxides and nitrides because they are halide-free and more reactive than chlorosilanes. However, the deposition of silicon nitride on oxide substrates still requires relatively high temperatures. We show here that for a process involving di<i>sec</i>-butylaminosilane and hydrazine, the insertion of Al from trimethyl aluminum allows the deposition of silicon nitride films at relatively low temperatures (250 °C). First-principles calculations reveal that the presence of Al increases the binding of molecular hydrazine, thereby effectively enhancing the reactivity of hydrazine with the silicon precursor during the atomic layer deposition process, which leads to nitrogen incorporation into silicon. However, the range of this enhancement is limited to ∼1 nm, requiring additional trimethylaluminum exposures to continue the Si<sub>3</sub>N<sub>4</sub> deposition.