Multi-head spatial atomic layer deposition: a robust approach for precise doping and nanolaminate fabrication in open-air environments

Abstract

Open-air manufacture of functional nanolaminates demands rapid and scalable methods that maintain nanoscale precision across individual layers. Conventional spatial atomic layer deposition (SALD) employs a single deposition head, and the concurrent exposure to mutually reactive precursors does not provide precise layer thickness accuracy nor sharp interfaces. This work addresses these challenges with an innovative multi-head SALD design. In this study, we introduced a novel multi-head SALD system comprising a uniform head for depositing 5 nm zinc oxide (ZnO) sublayers, while a combinatorial high-throughput head delivered wedge-like thickness gradient in aluminum oxide (Al₂O₃) sublayers, increasing gradually from 0 to approximately 6 nm along the substrate. Eight ZnO/Al₂O₃ bilayers (320 ALD cycles per material) were completed in open air at 200 °C. Transmission electron microscopy recorded highly sharp and reproducible layer-to-layer structures with thickness deviations of 0.3 nm; X-ray photoelectron spectroscopy verified the absence of undesirable aluminum contamination in the reference ZnO regions. With increasing Al₂O₃ thickness, surface roughness was reduced from 0.58 to 0.33 nm, ZnO (002) reflections broadened as crystallite size was confined, and Kelvin probe measurements showed a shift in work function values from 4.75 to 4.35 eV with Al₂O₃ passivation. This study demonstrates that the multi-head SALD method offers a robust platform for achieving precise multilayer control in open-air conditions, thereby paving the way for further innovations in materials research through optimized experimental conditions and combinatorial approaches.