Mixed Tin-Titanium Oxides by Atomic Layer Deposition on Planar Substrates: Physical and Electronic Structure

Mortelliti, Michael J.; Huang, Chiung-Wei; Atkin, Joanna M.; Dempsey, Jillian L.

doi:10.1016/j.apsusc.2021.151564

Title: Mixed Tin-Titanium Oxides by Atomic Layer Deposition on Planar Substrates: Physical and Electronic Structure

Journal Article · Tue Oct 12 00:00:00 EDT 2021 · Applied Surface Science

DOI:https://doi.org/10.1016/j.apsusc.2021.151564· OSTI ID:1976870

Mortelliti, Michael J. ^[1]; Huang, Chiung-Wei ^[1]; Atkin, Joanna M. ^[1]; Dempsey, Jillian L. ^[1]

University of North Carolina, Chapel Hill, NC (United States)

Ternary atomic layer deposition of Sn-doped TiO_x (Sn:TiO_x) and Ti-doped SnO_x (Ti:SnO_x) was performed using tetrakisdimethylamidotitanium (IV) and tin(IV) with water at 150 °C on (1 0 0) Si and quartz substrates. The physical structure of the films was investigated using scanning electron, atomic force, and Kelvin probe force microscopies as well as spectroscopic ellipsometry, Raman spectroscopy, and X-ray diffraction. All as-deposited films are amorphous and possessed flat and conformal topographies with low surface roughness (<1 nm). Annealed Sn:TiO_x and Ti:SnO_x crystallize into the tetragonal anatase TiO₂ and cassiterite SnO₂ structures, respectively, without large variations to the film topography. The chemical composition of the as-deposited and annealed films was investigated through X-ray photoelectron spectroscopy. While dopants are homogenously mixed, the ternary ALD to form Sn:TiO_x and Ti:SnO_x surprisingly does not follow the rule of mixtures, despite similarities in both the growth rates of binary SnO_x and TiO_x and the precursors used. This finding is also supported by spectroscopic ellipsometry. Here, we postulate the deviation from the rule of mixtures is due to non-ideal surface chemistry of the binary ALD of SnO_x. The optical bandgap of all films was quantified by the Tauc analysis and the valence band position was investigated by valence band X-ray photoelectron spectroscopy. Intra-bandgap states above the valence band maximum were observed for as-deposited Ti:SnO_x and Sn:TiO_x and ascribed to 5 s states from Sn²⁺ ions. The presence of these intra-bandgap states induces enhanced visible absorption and bathochromic shifts to the apparent bandgap for all as-deposited films. Annealing the films removes the intra-bandgap states and increases the optical bandgap. Simplified band diagrams created using the data available demonstrated that the conduction and valence band positions did not vary between the positions of pure TiO₂ or SnO₂ with monotonic increases to the dopant incorporation.

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Research Organization:: University of North Carolina, Chapel Hill, NC (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC0001011

OSTI ID:: 1976870

Journal Information:: Applied Surface Science, Vol. 573, Issue C; ISSN 0169-4332

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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