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本文基于第一性原理方法研究了非晶态二氧化硅中性氧空位缺陷及其与氢原子的反应机理。结果显示，非晶态二氧化硅中存在5种稳定中性氧空位缺陷构型，相应的缺陷形成能与缺陷硅原子间距呈现显著正相关关系。其中，VD构型因形成能最低可能是辐照或制备过程中的主要缺陷，VF和VB构型的费米接触与Eγ′中心相近，而VD、VBP4和VDSi构型因电子成对存在导致费米接触为零。氢原子与中性氧空位缺陷通过形成Si-H键或硅羟基两种钝化方式可产生两类共7种中性氢化氧空位缺陷。电子定域化函数与EPR模拟分析发现，VHBB和VHBM构型与Eγ′中心的EPR参数高度接近，表明氢钝化过程可能干扰E′中心的识别。VBBOH构型中硅羟基的生成可为氧化层和界面处水分子的形成提供理论依据。研究获得了氢诱导缺陷跨网格迁移以及生成硅羟基的路径，并揭示了氢原子具有钝化原始缺陷和诱发次生缺陷的双重作用。这些发现可为双极型器件低剂量率辐射损伤增强效应提供微观机理解释。Amorphous silica (a-SiO2), with excellent insulating properties, uniform disordered structure and good thermal stability, is the preferred material for field oxide layers, gate insulation layers and passivation layers in numerous semiconductor devices. However, in space environments, oxygen vacancies resulted from high-energy particle radiation and their interactions with hydrogen atoms in a-SiO2 could lead to enhanced low-dose-rate sensitivity, potentially causing threshold voltage shifts and leakage current increases in semiconductor devices. These seriously threaten the operation safety of spacecraft, and the exploration of related reaction mechanisms is crucial. A first-principles calculation is employed to investigate the neutral oxygen vacancies in amorphous silica and their reaction mechanisms with hydrogen atoms. Five types of neutral oxygen vacancies are identified, namely VD, VB, VF, VBP4 and VDSi configurations. A significant positive correlation is observed between the defect formation energy and the distance between two defect silicon atoms. The VD configuration may become the major defect type in irradiation or fabrication due to the lowest defect formation energy. VF and VB configurations display comparable Fermi contacts to those of Eγ′ centers. The presence of electron pairs leads to zero fermi contacts in VD, VBP4 and VDSi configurations. To reactions between oxygen vacancies and hydrogen atoms, the previous investigations often pay more attention to the reactions with hydrogen atoms at the middle-sites of oxygen vacancies. And, a critical characteristic of the disordered a-SiO2 structure is neglected by this approach: the reactions may extend into the neighboring network and occur at side-sites of oxygen defects. For a full understanding of actual reactions, both the middle-sites and side-sites are considered for hydrogen atoms in present investigations. It’s revealed that hydrogen atoms passivate neutral oxygen vacancies through two distinct mechanisms: Si-H bond formation or silanol group generation. These processes yield two classes of neutral hydrogenated oxygen vacancies, VH and VOH configurations, which can be further classified into seven distinct configurations based on the orientation of dangling bonds and Si-H bonds. By combining the analyses of ELF maps and EPR simulations, it is demonstrated that VBB H and VBM H configurations have comparable EPR parameters to those of Eγ′ center, implying that hydrogen passivation processes may interfere with the identification of E′ center. The formation of silanol group in VBB OH configuration provides theoretical bases for explaining water molecules formation within oxide layers and at interfaces. This study elucidates the hydrogen-induced crossnetwork migration and silanol group formation pathway, collectively revealing the dual role of hydrogen in passivating defects and inducing secondary defects. A microscopic explanation is derived from these findings for the enhanced low dose rate sensitivity in bipolar devices.
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Keywords:
- Neutral oxygen vacancy /
- hydrogen atom /
- passivation /
- first-principles
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