Bimolecular Reaction Mechanism in the Amido Complex-Based Atomic Layer Deposition of HfO2

Giulio D'acunto, Roman Tsyshevsky, Payam Shayesteh, Jean Jacques Gallet, Fabrice Bournel, François Rochet, Indiana Pinsard, Rainer Timm, Ashley R. Head, Maija Kuklja, Joachim Schnadt

Forskningsoutput: TidskriftsbidragArtikel i vetenskaplig tidskriftPeer review

Sammanfattning

The surface chemistry of the initial growth during the first or first few precursor cycles in atomic layer deposition is decisive for how the growth proceeds later on and thus for the quality of the thin films grown. Yet, although general schemes of the surface chemistry of atomic layer deposition have been developed for many processes and precursors, in many cases, knowledge of this surface chemistry remains far from complete. For the particular case of HfO2 atomic layer deposition on a SiO2 surface from an alkylamido-hafnium precursor and water, we address this lack by carrying out an operando atomic layer deposition experiment during the first cycle of atomic layer deposition. Ambient-pressure X-ray photoelectron spectroscopy and density functional theory together show that the decomposition of the metal precursor on the stoichiometric SiO2 surface in the first half-cycle of atomic layer deposition proceeds via a bimolecular reaction mechanism. The reaction leads to the formation of Hf-bonded methyl methylene imine and free dimethylamine. In addition, ligand exchange takes place involving the surface hydroxyls adsorbed at defect sites of the SiO2 surface.

Originalspråkengelska
Sidor (från-till)529-538
TidskriftChemistry of Materials
Volym35
Nummer2
Tidigt onlinedatum2022
DOI
StatusPublished - 2023

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