Ab Initio Investigation of Surface Chemistry of Alumina ALD on Hydroxylated γ-Alumina Surface

Aditya Shankar Sandupatla, Konstantinos Alexopoulos, Marie Françoise Reyniers, Guy B. Marin

Research output: Contribution to journalArticlepeer-review

15 Scopus citations

Abstract

Atomic layer deposition (ALD) of alumina using trimethyl aluminum (TMA) and water on amorphous alumina is analyzed using periodic-dispersion corrected DFT calculations. The energetics of the investigated reactions suggest that monomethyl aluminum (MMA) is the most abundant reaction intermediate at ALD operating conditions. The dominant reaction path toward the methylation of the surface is found to be adsorption of TMA on bridge oxygen via Lewis acid-base complex formation followed by ligand exchange reactions (LERs) with hydroxyls and surface water in its vicinity. Further adsorption and LERs of TMA leads to a saturated methylated surface (∼6.4 CH3 nm-2) which is in agreement with experimental observations and infrared spectra. The surface restructuring that is observed in almost all the reactions investigated seems to play an important role in the formation of conformal alumina films.

Original languageEnglish (US)
Pages (from-to)13050-13061
Number of pages12
JournalJournal of Physical Chemistry C
Volume119
Issue number23
DOIs
StatePublished - Jun 11 2015

All Science Journal Classification (ASJC) codes

  • Electronic, Optical and Magnetic Materials
  • Energy(all)
  • Physical and Theoretical Chemistry
  • Surfaces, Coatings and Films

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