Hydrogen passivation mechanism and reaction pathways of neutral oxygen vacancies in amorphous silica

WANG Yuqi; ZHAO Yaolin; YU Chenxi; ZHANG Jun

doi:10.7498/aps.74.20250831

Abstract
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 many semiconductor devices. However, in space environments, the oxygen vacancies generated by high-energy particle radiation and their interaction with hydrogen atoms in a-SiO₂ can lead to enhanced low-dose-rate sensitivity, potentially causing threshold voltage to shift and leakage current to increase in semiconductor devices. These seriously threaten the operation safety of spacecraft, and the exploration of related reaction mechanisms is crucial. The neutral oxygen vacancies in amorphous silica and their reaction mechanism with hydrogen atoms are investigated using first-principles calculations. Five types of neutral oxygen vacancies are identified, namely $ {\mathrm{V}}_{\mathrm{D}} $, $ {\mathrm{V}}_{\mathrm{B}} $, $ {\mathrm{V}}_{\mathrm{F}} $, $ {\mathrm{V}}_{\mathrm{B}\mathrm{P}4} $ and $ {\mathrm{V}}_{\mathrm{D}\mathrm{S}\mathrm{i}} $ configurations. A significant positive correlation is observed between the defect formation energy and the distance between two defective silicon atoms. Due to the lowest defect formation energy, the $ {\mathrm{V}}_{\mathrm{D}} $ configuration may become the main type of defect in irradiation or fabrication.$ {\mathrm{V}}_{\mathrm{F}} $ and $ {\mathrm{V}}_{\mathrm{B}} $ configurations show that Fermi contacts are comparable to those of $ {\mathrm{E}}_{\mathrm{\gamma }}' $ centers. The presence of electron pairs leads to zero fermi contacts in $ {\mathrm{V}}_{\mathrm{D}} $, $ {\mathrm{V}}_{\mathrm{B}\mathrm{P}4} $ and $ {\mathrm{V}}_{\mathrm{D}\mathrm{S}\mathrm{i}} $ configurations. Previous studies have often focused more on the reaction between oxygen vacancies and hydrogen atoms at the middle-sites of oxygen vacancies. And, a key characteristic of the disordered a-SiO₂ structure is that this method ignores the structure: the reaction may extend to the neighboring networks and occur at the 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. The research shows that hydrogen atoms passivate neutral oxygen vacancies through two different mechanisms: the formation of Si-H bonds and the generation of silanol groups. These processes generate two types of neutral hydrogenated oxygen vacancies, $ {\mathrm{V}}^{\mathrm{H}} $ and $ {\mathrm{V}}^{\mathrm{O}\mathrm{H}} $ configurations, which can be further divided into seven different 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 $ {\mathrm{V}}_{\mathrm{B}\mathrm{B}}^{\mathrm{H}} $ and $ {\mathrm{V}}_{\mathrm{B}\mathrm{M}}^{\mathrm{H}} $ configurations have EPR parameters comparable to those of $ {\mathrm{E}}_{\mathrm{\gamma }}' $ center, indicating that hydrogen passivation processes may interfere with the identification of $ {\mathrm{E}}' $ center. The formation of silanol group in $ {\mathrm{V}}_{\mathrm{B}\mathrm{B}}^{\mathrm{O}\mathrm{H}} $ configuration provides theoretical bases for explaining water molecules formation within oxide layers and at interfaces. This study elucidates the pathways of hydrogen-induced cross-network migration and silanol group formation, jointly revealing the dual role of hydrogen in passivating defects and inducing secondary defects. A microscopic explanation for the increased sensitivity to low dose rates in bipolar devices is derived from these findings.

Keywords:
neutral oxygen vacancy /

hydrogen atom /

passivation /

first-principles
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图 1 (a) 无缺陷a-SiO₂模型^[27](红色为氧原子、黄色硅原子); (b) Si—O键长示意图; (c) a-SiO₂键角分布

Figure 1. (a) Model of defect-free a-SiO₂ ^[27](red spheres, oxygen atoms; yellow spheres, silicon atoms); (b) schematic diagram of the Si—O bond length; (c) bond angle distribution in a-SiO₂.

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图 2 a-SiO₂中5种中性氧空位缺陷的典型结构(红色为氧原子、黄色硅原子)和ELF图

Figure 2. Typical configurations and ELF maps of five types of neutral oxygen vacancies in a-SiO₂ (red spheres, oxygen atoms; yellow spheres, silicon atoms).

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图 3 中性氧空位缺陷的缺陷形成能

Figure 3. Defect formation energy of neutral oxygen vacancies.

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图 4 a-SiO₂中7种中性氢化氧空位缺陷的典型结构(红色为氧原子、黄色硅原子、白色为氢原子)

Figure 4. Seven typical configurations of neutral hydrogen-passivated oxygen vacancies in a-SiO₂ (red spheres, oxygen atoms; yellow spheres, silicon atoms; white spheres, hydrogen atoms).

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图 5 a-SiO₂中7种中性氢化氧空位缺陷的ELF图

Figure 5. ELF maps of seven neutral hydrogen-passivated oxygen vacancies in a-SiO₂.

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图 6 (a) $ {\mathrm{V}}_{\mathrm{D}} $和(b) $ {\mathrm{V}}_{\mathrm{B}} $构型与氢原子的反应路径和能量曲线

Figure 6. Reaction pathways and energy curves of (a) $ {\mathrm{V}}_{\mathrm{D}} $ and (b) $ {\mathrm{V}}_{\mathrm{B}} $ configurations with hydrogen atoms.

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图 7 (a) $ {\mathrm{V}}_{\mathrm{F}} $和(b) $ {\mathrm{V}}_{\mathrm{B}\mathrm{P}4} $构型与氢原子的反应路径和能量曲线

Figure 7. Reaction pathways and energy curves of (a) $ {\mathrm{V}}_{\mathrm{F}} $ and (b) $ {\mathrm{V}}_{\mathrm{B}\mathrm{P}4} $ configurations with hydrogen atoms.

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图 8 $ {\mathrm{V}}_{\mathrm{D}\mathrm{S}\mathrm{i}} $构型与氢原子的反应路径和能量曲线

Figure 8. Reaction pathway and energy curve of $ {\mathrm{V}}_{\mathrm{D}\mathrm{S}\mathrm{i}} $ configuration with a hydrogen atom.

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表 1 五种中性氧空位缺陷的结构参数

Table 1. Structural parameters of five types of neutral oxygen vacancies.

种类	数量	平均$ {D}_{\mathrm{S}\mathrm{i}1-\mathrm{S}\mathrm{i}2} $ /Å	平均Si—O 键长/Å		平均O—Si—O 键角/(°)
种类	数量	平均$ {D}_{\mathrm{S}\mathrm{i}1-\mathrm{S}\mathrm{i}2} $ /Å	Si1	Si2	Si1	Si2
$ {\mathrm{V}}_{\mathrm{D}} $	24	2.42	1.66	1.66	106.95	107.34
$ {\mathrm{V}}_{\mathrm{F}} $	7	4.19	1.66	1.66	108.52	108.91
$ {\mathrm{V}}_{\mathrm{B}} $	14	4.81	1.66	1.66	109.31	108.19
$ {\mathrm{V}}_{\mathrm{B}\mathrm{P}4} $	2	5.32	1.80	1.60	96.27	114.07
$ {\mathrm{V}}_{\mathrm{D}\mathrm{S}\mathrm{i}} $	1	3.53	1.71	1.66	99.67	111.63

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表 2 中性氧空位缺陷和中性氢化氧空位缺陷的平均费米接触和g因子

Table 2. Average Fermi contacts and g values of neutral oxygen vacancies and neutral hydrogen-passivated oxygen vacancies.

缺陷构型	费米接触/mT		g₁	g₂	g₃
缺陷构型	Si1	Si2	g₁	g₂	g₃
$ {\mathrm{V}}_{\mathrm{B}} $	–38.10	–40.69	2.0006	1.9988	1.9981
$ {\mathrm{V}}_{\mathrm{F}} $	–41.79	–42.95	2.0005	1.9986	1.9979
$ {\mathrm{V}}_{\mathrm{B}\mathrm{B}}^{\mathrm{H}} $	–39.29	–0.00	2.0017	2.0006	2.0002
$ {\mathrm{V}}_{\mathrm{B}\mathrm{F}}^{\mathrm{H}} $	–0.03	–45.07	2.0017	2.0002	1.9998
$ {\mathrm{V}}_{\mathrm{F}\mathrm{B}}^{\mathrm{H}} $	–44.27	–0.12	2.0017	2.0003	2.0000
$ {\mathrm{V}}_{\mathrm{F}\mathrm{F}}^{\mathrm{H}} $	–16.55	–41.14	2.0014	2.0002	1.9997
$ {\mathrm{V}}_{\mathrm{B}\mathrm{M}}^{\mathrm{H}} $	–0.01	–0.27 (–41.72^a)	2.0016	2.0004	2.0001
$ {\mathrm{V}}_{\mathrm{D}\mathrm{S}\mathrm{i}}^{\mathrm{H}} $	–22.89	–0.02	2.0021	2.0020	2.0005
$ {\mathrm{V}}_{\mathrm{B}\mathrm{B}}^{\mathrm{O}\mathrm{H}} $	–43.75	–0.60	2.0016	2.0005	1.9998
注: ^a 表示Si4费米接触.

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