Quantum Chemical Study of Zirconium Oxide Deposition on the Si(100)−(2×1) Surface

Zirconium oxide (ZrO 2 ) deposition on the Si(100)-(2×1) surface is investigated using density functional theory (DFT). The reactants investigated in this study are ZrCl 4 and H 2 O. The atomistic mechanisms of the two different deposition cycles are investigated: (1) First, ZrCl 4 is deposited on the clean Si(100)-(2×1) surface. Upon adsorption, ZrCl 4 is shown to dissociate into ZrCl 3 (a) and Cl(a) with an activation barrier that is below the entrance channel. Next, water is deposited and reactions on the Si−Cl* and Zr−Cl* surface sites are investigated, where the asterisks denote the surface species. Alternatively, (2) H 2 O is first deposited on the Si(100)-(2×1) surface. As previously determined, we also find that H 2 O dissociates into OH(a) and H(a) upon adsorption. Subsequent reactions of ZrCl 4 with the resulting Si−OH* and Si−H* sites are then investigated. Reactions on Si−H* sites also provide insight into the growth on hydrogen-terminated Si surfaces. Upon investigation of the two different deposition cycles, the structure of the interfacial layer between silicon and zirconium oxide is then investigated.