Plasma-assisted thermal atomic layer etching for palladium and surface structure analysis with density-functional theory
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초록

The plasma-assisted thermal atomic layer etching (ALE) process was performed on the palladium (Pd) using sequential, self-limiting thermal reactions with surface chlorination using Cl<inf>2</inf> plasma and removal with NH<inf>3</inf> ligand addition. The formation of PdCl<inf>2</inf> layer was confirmed with x-ray photoelectron spectroscopy (XPS) in the chlorination step. The chlorination depth was saturated to 16 Å after 30 s of Cl<inf>2</inf> plasma exposure at 150 °C. The etching was performed via NH<inf>3</inf> ligand addition above 100 °C. The etch per cycle (EPC) was saturated at 16 Å/cycle after 30 s of Cl<inf>2</inf> plasma exposure and 30 s of NH<inf>3</inf> ligand addition at 150 ∼ 200 °C. Surface chlorine residues after ALE were less than 1 % under process conditions with self-limiting characteristics. The surface roughness increased from 0.24 to 0.52 nm after 20 ALE cycles. No crystallinity changes after ALE, but the individual peak areas decreased differently by 61 % for Pd(111), 56 % for Pd(100), 66 % for Pd(110), and 94 % for Pd(311). Density functional theory (DFT) calculations showed that Pd(311) had the lowest reaction energy of −0.576 eV. The reaction product was proposed as trans-Pd(NH<inf>3</inf>)<inf>2</inf>Cl<inf>2</inf>, showing the lowest reaction energy yield of 0.26 eV when NH<inf>3</inf> is adsorbed on the chlorinated Pd surface. © 2025 Elsevier B.V., All rights reserved.

키워드

Atomic layer etching (ALE)CrystallinityDensity-functional theory (DFT)PalladiumSurface roughnessHYDROGEN SENSORSOXIDATIONNANOSTRUCTURESNANOPARTICLESPRESSUREPD
제목
Plasma-assisted thermal atomic layer etching for palladium and surface structure analysis with density-functional theory
저자
Kang, HojinHuh, EugeneCho, AhyeonCho, SooyeonLee, SangheonChae, Heeyeop
DOI
10.1016/j.apsusc.2025.164925
발행일
2026-02-28
유형
Article
저널명
Applied Surface Science
719