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中国物理学会期刊

单层Z-Bi2O2Se本征点缺陷及光电性能

CSTR: 32037.14.aps.74.20241701

Intrinsic point defects and optoelectronic properties in monolayer Z-Bi2O2Se

CSTR: 32037.14.aps.74.20241701
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  • 采用基于密度泛函理论的第一性原理和非平衡格林函数方法, 系统研究了单层拉链型硒氧化铋(Z-Bi2O2Se)中空位、反位和吸附点缺陷的结构、电子和光电性质. 通过在不同生长环境下形成能的计算发现, 点缺陷O' 空位, O取代Se反位、Se 吸附Bi'-Bi'-Se和Bi-Bi-Se穴位相对容易形成; 电子态密度及形成能的计算结果显示, O' 空位、Se吸附Bi'-Bi'-Se和Bi-Bi-Se穴位属于深能级n型掺杂. 此外, 沿平行和垂直拉链方向分别构建了基于单层Z-Bi2O2Se的器件, 其光电性能表现出明显的各向异性. 点缺陷的引入降低了体系对称性, 使其光电流在可见光区和紫外光区显著增大, 各向异性仍然存在. 点缺陷对器件消光比的影响同时取决于点缺陷类型及光子能量, 通过选择点缺陷在特定光子能量的照射可以有效提高器件的偏振灵敏度. 本文研究结果对深入认识二维Bi2O2Se结构及其性能提供理论指导.

     

    The novel layered semiconductor material bismuth oxyselenide (Bi2O2Se) exhibits exceptional properties such as thickness-dependent bandgap, superior electron mobility, compatibility with various materials, and stability under ambient conditions. The zipper-type two-dimensional Bi2O2Se (Z-Bi2O2Se) is a newly proposed structure based on theoretical studies of material surface dissociation mechanisms. However, current understanding of this structure still mainly focuses on fundamental investigations of electronic properties such as band structures. Intrinsic point defects, which are inevitable during material synthesis and operational environments, significantly influence the physical characteristics of materials and ultimately dictate device performance. In this work, we conduct an in-depth exploration of intrinsic point defects in the material. Using first-principles calculations based on density functional theory (DFT) and non-equilibrium Green’s function (NEGF) methods, we systematically investigate the structural, electronic, and optoelectronic properties of vacancies, antisites, and adatom point defects in Z-Bi2O2Se. First, the formation energy calculations under different growth conditions reveal that o'vacancy, Se replaced by O, Se adsorption on “Bi'-Bi'-Se” and “Bi-Bi-Se” hollow sites are relatively easy to form. The density of states (DOS) and formation energy shows that o'vacancy, Se adsorption on “Bi'-Bi'-Se” and “Bi-Bi-Se” hollow sites tend to lose electrons and become positively charged. Their donor levels are located at 0.78 eV, 0.01 eV, and 0.07 eV above the valence band maximum (VBM), but well below the conduction band minimum (CBM), indicating deep-level n-type doping characteristics. Furthermore, devices based on monolayer Z-Bi2O2Se along the parallel (Z//) direction and perpendicular (Z) direction of the “zipper” structure are constructed to investigate the influence of intrinsic point defects on optoelectronic performance. The results show that for pristine materials, the photocurrent of Z-perfect in the visible and ultraviolet regions is two orders of magnitude smaller than that of Z//-perfect, demonstrating significant anisotropy. The introduction of point defects reduces system’s symmetry, leading to a remarkable enhancement of photocurrent in both devices in these spectral regions. Notably, in the Z direction, the point defects induce the photocurrent to increase by three orders of magnitude. However, the photocurrent remains relatively small compared with that in Z// direction, indicating persistent anisotropy. The influence of point defects on the extinction ratio depends on both defect types and photon energy. By selecting specific point defects under irradiation at targeted photon energy, the polarization sensitivity of devices can be effectively improved. These findings provide theoretical guidance for deepening the understanding of the electronic structure and optoelectronic properties of two-dimensional Z-Bi2O2Se.

     

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