Density functional theory predictions of the composition of atomic layer deposition-grown ternary oxides

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Murray, Ciarán A.
Elliott, Simon D.
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American Chemical Society
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The surface reactivity of various metal precursors with different alkoxide, amide, and alkyl ligands during the atomic layer deposition (ALD) of ternary oxides was determined using simplified theoretical models. Quantum chemical estimations of the Bronsted reactivity of a metal complex precursor at a hydroxylated surface are made using a gas-phase hydrolysis model. The geometry optimized structures and energies for a large suite of 17 metal precursors (including cations of Mg, Ca, Sr, Sc, Y, La, Ti, Zr, Cr, Mn, Fe, Co, Ni, Cu, Zn, Al, and Ga) with five different anionic ligands (conjugate bases of tert-butanol, tetramethyl heptanedione, dimethyl amine, isopropyl amidine, and methane) and the corresponding hydrolyzed complexes are calculated using density functional theory (DFT) methods. The theoretically computed energies are used to determine the energetics of the model reactions. These DFT models of hydrolysis are used to successfully explain the reactivity and resulting stoichiometry in terms of metal cation ratios seen experimentally for a variety of ALD-grown ternary oxide systems.
Density functional theory , Ternary oxides , Stoichiometry , Metal precursors , Ligand , Atomic layer deposition (ALD)
MURRAY, C. & ELLIOTT, S. D. 2013. Density Functional Theory Predictions of the Composition of Atomic Layer Deposition-Grown Ternary Oxides. ACS Applied Materials & Interfaces, 5, 3704-3715.
© 2013 American Chemical Society. This document is the Accepted Manuscript version of a Published Work that appeared in final form in ACS Applied Materials & Interfaces copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see