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DOE OSTI · 3372185

Site-specific surface reactivity on MgO for atomic layer deposition via selective hydration

Yan, Chang [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000247061236)·Xu, Jiayi [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000317636251)·Muir, Mark [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000318900579)·Dua, Asare [Illinois Institute of Technology, Chicago, IL (United States)] (ORCID:0000000244303674)·Hock, Adam [Illinois Institute of Technology, Chicago, IL (United States)]·Martinson, Alex B.F. [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000339161672)·Liu, Cong [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000221455034)
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Abstract

Atomic layer deposition (ALD) is a powerful technique for thin film synthesis, offering atomic-scale precision and conformality. While ALD of MgO has been widely studied for applications in energy storage and microelectronics, its potential as surface on which deposition may be selective and defects repaired remains underexplored. Here, we present a combined theoretical and experimental investigation of MgO surface hydration and its implications for targeted ALD growth using water and dimethyl aluminum isopropoxide (DMAI) as reactants. We perform density functional theory (DFT) calculations to examine molecular and dissociative H 2 O adsorption on MgO (100) terraces and step-edge sites, including pristine surfaces and those with Mg/O vacancies. Reaction Gibbs free energies are calculated under various conditions to quantify surface reactivity. Our findings reveal facet- and defect-dependent hydration behaviors that align with experimental ALD growth trends on MgO (100). This study provides a molecular-level understanding of MgO surface chemistry critical for optimizing ALD processes for thin film growth and defect repair.

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRYAtomic layer depositionDensity Functional TheoryMetal oxidesSurface hydration

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Yan, Chang [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000247061236), Xu, Jiayi [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000317636251), Muir, Mark [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000318900579), Dua, Asare [Illinois Institute of Technology, Chicago, IL (United States)] (ORCID:0000000244303674), Hock, Adam [Illinois Institute of Technology, Chicago, IL (United States)], Martinson, Alex B.F. [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000339161672), Liu, Cong [Argonne National Laboratory (ANL), Lemont, IL (United States)] (ORCID:0000000221455034). 2025-12-24. Site-specific surface reactivity on MgO for atomic layer deposition via selective hydration. https://doi.org/10.1016/j.apsusc.2025.165698

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