通过XPS/HAXPES弥合化学状态分析的经典与量子解释以解析非晶氧化铝薄膜的短程有序
Bridging classical and quantum interpretation of chemical state analysis by XPS/HAXPES to resolve short-range order in amorphous alumina films
AI总结：
本研究整合XPS/HAXPES光谱、机器学习分子动力学模拟、DFT计算及经典静电建模，揭示ALD非晶氧化铝的短程有序结构与化学性质，为宽带隙非晶氧化物的XPS谱解析提供新途径。
摘要：
由于实验室光谱技术的局限性，探测宽带隙非晶氧化物薄膜的局部结构和化学性质仍具挑战性。本工作整合X射线光电子能谱（XPS）、硬X射线光电子能谱（HAXPES）、基于机器学习原子间势的分子动力学模拟、密度泛函理论（DFT）计算，以及Al原子终态芯电离效应的经典静电建模，以揭示原子层沉积（ALD）制备的非晶氧化铝多晶型的结构和化学性质。使用Delta Kohn-Sham方法的DFT计算支持了终态效应的解释并验证了静电模型假设。测量的俄歇参数偏移被解释为原子外弛豫能，显示出对局部配位环境的敏感性。研究发现结构无序和热涨落主导原子外弛豫能的分布，表明低温XPS可分离并揭示非晶氧化物的本征结构基元。模拟加热和退火表明，俄歇参数偏移可作为H过饱和ALD非晶氧化铝中相分解的指标。这些发现为非晶宽带隙氧化物中XPS谱的全面解释和预测建模提供了途径。
英文摘要：
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 Delta Kohn-Sham method supported the interpretation of final-state effects and validated electrostatic model assumptions. Shifts in the measured Auger parameter were interpreted as extra-atomic relaxation energies, revealing sensitivity to the local coordination environment. Structural disorder and thermal fluctuations were found to govern the distribution of extra-atomic relaxation energies, suggesting that cryo-XPS can isolate and reveal intrinsic structural building blocks of amorphous oxides. Simulated heating and annealing demonstrated that Auger parameter shifts can serve as indicators of phase decomposition in H-supersaturated ALD amorphous alumina. These findings provide a pathway for comprehensive interpretation and predictive modeling of XPS spectra in amorphous wide-bandgap oxides.
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