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大直径直拉单晶硅(Cz-Si)已成为微电子器件和太阳能电池的主流衬底材料。作为直拉单晶硅中最不可避免的杂质，氧杂质倾向于在晶体生长以及后续制程中形成氧关缺陷,这极大地影响了器件性能。目前，产业对大直径直拉单晶硅质量提出了更高的要求，这亟须对大直径直拉单晶硅中氧关缺陷有更深入的认知。本文围绕大直径直拉单晶硅中最为主要的几种氧关缺陷(氧关复合体、氧热施主、氧沉淀)研究现状，综述了氧关缺陷的形成机制以及电学性质。讨论了大直径直拉单晶硅中氧关缺陷的研究展望以及控制策略，以期为高质量大直径直拉单晶硅的生长和氧关缺陷控制提供理论指导。
Abstract：Large-diameter Czochralski silicon(Cz-Si), particularly 300 mm wafer, becomes a dominant substrate material for integrated circuits(ICs) and replacs smaller diameters in the photovoltaic(PV) industry. Oxygen, introduced primarily through quartz crucible erosion during crystal growth, is one of the most inevitable and technologically critical impurity in Cz-Si. During crystal growth cooling and subsequent device processing, interstitial oxygen(Oi) atoms aggregate to form various electrically active oxygen-related defects, significantly degrading device performance. Oxygen precipitates contribute to a crucial role of internal gettering(IG) in IC industry. Understanding and controlling these defects are paramount for advancing both microelectronic and solar cell technologies. This review comprehensively analyzes the formation mechanisms, electrical properties, and control strategies for major oxygen-related defects in large-diameter Cz-Si. This review firstly represents the fundamental properties of oxygen impurities in Cz-Si, including the equilibrium solubility and the diffusion coefficient derived from plenty of works. Enhanced diffusion phenomenon was reported at 500–700 ℃. Some models like the dioxygen(O2i), oxygen–vacancy(O–V), and oxygen-self-interstitial(O–I) complexes were proposed to explain this phenomenon. Thermal donors(TDs) generate at 400–500 ℃ via oxygen clustering. The formation kinetics are comprehensively investigated. TDs exhibit double donor properties and have an impact on the carrier concentration of Cz-Si. TDs can be annealed out at 650 ℃, while prolonged annealing can originate new donors(NDs). The agglomeration of oxygen can generate oxygen precipitates(OPs). Some nucleation peaks at 650–750 appear in high [O℃i] and crystal head regions. The growth(at 850–1050 ℃) is diffusion-limited. The morphology depends critically on annealing temperature and supersaturation. For the electrical properties, OPs serve as strong recombination centers, drastically reducing minority carrier lifetime and increasing reverse leakage current in devices. In IC industry, OPs and their secondary defects serve as internal gettering sites, which play a crucial role on the formation of denude zone. Oxygen-related complexes consist of oxygen atoms and other impurity atoms. For the acceptor-oxygen complexes, the Boron–Oxygen(B–O) complex is a primary cause of light-induced degradation(LID) in p-type Cz-Si solar cells. It requires both B and O, which exhibits a metastable degradation(i.e., activated by excess carriers, activation energy of 0.2–0.4 eV) and a stable recovery(i.e., activation energy of 1.3 eV). The widely accepted B_sO2i model features bistable configurations( "Annealed" and "Degraded" states). A "Third State"(fully recovered, immune to further degradation) is also identified. Al_sO2i, Ga_sO2i and In_sO2i are identified, exhibiting no obvious degradation. Thus, Ga doping is widely adopted as impurities in engineering to suppress LID. For the intrinsic point defect-oxygen complexes, oxygen effectively traps vacancies and forms vacancy–oxygen(VOn, n= 1–6) complexes. VO(A-center, EC–0.17 eV) and VO are significant recombination centers. VO dominates after high-temperature RTA(at 1250–1400 ℃). VO complexes, especially VO, act as potent heterogeneous nucleation sites for oxygen precipitates, which are crucial for internal gettering in ICs. Isoelectronic dopants(Ge, Sn, Pb) and nitrogen affect VOn formation and stability. Light impurities-oxygen complexes mainly focus on Nitrogen—Oxygen(N—O) and Carbon—Oxygen(C—O) complexes. Nitrogen forms electrically inactive complexes like N_2O and N_2O2. N also forms a shallow donor NOx(i.e., ionization energy 34–37 meV, IR peaks 190–270 cm1). Carbon enhances oxygen precipitate, which can originate from the formation of C–O complexes. Summary and Prospects The key formation mechanisms and electrical properties of oxygen-related defects remain some challenges. The crystal growth for 300 mm wafers involves complex multi-physics(i.e., thermal, flow, electromagnetic fields) in large systems(i.e., 34–37 in crucibles, 300–450 kg charge). Maintaining radial uniformity is difficult due to the V/G criterion(where V is pull rate, and G is axial temperature gradient). Deviations lead to vacancy-rich(V) or interstitial-rich(I) regions, with a transition zone prone to forming a ring of "P-band" native oxygen-related defects. This causes a radial non-uniformity in oxygen clustering during device processing, concerning the radial defect non-uniformity and nucleation anomalies in 300 mm crystals. We should also focus on the interaction between oxygen-related defects and metallic impurities in Cz-Si used for solar cells. We can benefit from effective control of oxygen-related defect in Large-diameter Cz-Si. The effective control requires a multi-pronged approach, i.e., sophisticated crystal growth optimization(thermal/flow fields, magnetic fields, doping), strategic impurity engineering(nitrogen, isovalent dopants), and tailored thermal processing. A further research into defect interactions, advanced characterization, and multi-scale modeling is essential for pushing the performance limits of next-generation silicon devices.
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基本信息:
DOI：10.14062/j.issn.0454-5648.20250221
中图分类号:TN304.12
引用信息:
[1]吴若楷,余学功,杨德仁.大直径直拉硅单晶中的氧关缺陷[J].硅酸盐学报,2025,53(12):3506-3519.DOI:10.14062/j.issn.0454-5648.20250221.
基金信息:
国家自然科学基金(62025403)