Bridging classical and quantum interpretation of chemical state analysis by XPS/HAXPES to resolve short-range order in amorphous alumina films
Simon Gramatte, Xing Wang, Michael Alejandro Hernández Bertrán, Claudia Cancellieri, Giovanni Pizzi, Deborah Prezzi, Iurii Timrov, Olivier Politano, Ivo Utke, Lars P. H. Jeurgens, Vladyslav Turlo
TL;DR
This study combines XPS/HAXPES and simulations to understand the structure and chemistry of amorphous alumina films.
Contribution
The integration of XPS/HAXPES with advanced simulations provides new insights into the local structure of amorphous oxides.
Findings
Auger parameter shifts reveal local coordination environments in amorphous alumina.
Cryo-XPS can isolate intrinsic structural building blocks in amorphous oxides.
Thermal fluctuations and structural disorder influence extra-atomic relaxation energies.
Abstract
Probing the local structure and chemistry of wide-bandgap amorphous oxide thin films remains challenging due to the limitations of lab-based spectroscopy. This work integrates X-ray photoelectron spectroscopy (XPS), hard X-ray photoemission spectroscopy (HAXPES), molecular dynamics simulations using machine-learning interatomic potentials, density-functional theory (DFT) calculations, and classical electrostatic modeling of final-state core-ionization effects in Al atoms to uncover the structure and chemistry of amorphous alumina polymorphs made with atomic layer deposition (ALD). DFT calculations using the ΔKohn–Sham method supported the interpretation of final-state effects and validated electrostatic model assumptions. Shifts in the measured Auger parameters were interpreted as extra-atomic relaxation energies, revealing sensitivity to the local coordination environment. Structural…
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Taxonomy
TopicsAdvanced ceramic materials synthesis · Thermal Expansion and Ionic Conductivity · X-ray Diffraction in Crystallography