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设计二维半导体范德瓦耳斯异质结是一种实现多功能微电子器件的有效策略. 本文构筑了二维钙钛矿Cs3X2I9 (X = Bi, Sb)和铟锡InSe的范德瓦耳斯异质结Cs3X2I9/InSe. 基于密度泛函理论的第一性原理方法, 计算了其几何、电子结构、光学性质. 研究表明, 二维Cs3Bi2I9/InSe和Cs3Sb2I9/InSe异质结为II型能带排列, 且带隙分别为1.61 eV和1.19 eV, 可见光和紫外光范围内具有较高的吸收系数. 基于形变势理论和类氢原子模型的计算, 二维Cs3X2I9/InSe异质结显示了较高的激子结合能和电子迁移速率. 基于II型排列的能带结构和肖克利-奎伊瑟极限(Shockley-Queisser limit), 对比研究了光电转换效率. 此外, 进一步探究了双轴应变对二维Cs3X2I9/InSe异质结光电特性的调控和规律. 上述研究为未来设计高效的二维范德瓦耳斯光电子器件提供了理论依据.Two-dimensional semiconductor heterostructures have excellent physical properties such as high light absorption coefficients, large diffusion lengths, high carrier mobility rates, and tunable energy band structures, which have great potential in the field of optoelectronic devices. Therefore, designing two-dimensional (2D) semiconductor van der Waals heterostructures is an effective strategy for realizing multifunctional microelectronic devices. In this work, the 2D van der Waals heterostructure Cs3X2I9/InSe of non-lead Perovskite Cs3X2I9 and indium-tin InSe is constructed to avoid the toxicity and stability problems of lead-based Perovskites. The geometry, electronic structure, and optical properties are calculated based on the first-principles approach of density-functional theory. It is shown that the 2D Cs3Bi2I9/InSe and Cs3Sb2I9/InSe heterostructures are of type-II energy band arrangement and have band gaps of 1.61 eV and 1.19 eV, respectively, with high absorption coefficients in the visible range and UV range reaching to 5×105 cm–1. The calculation results from the deformation potential theory and the hydrogen-like atom model show that the 2D Cs3X2I9/InSe heterostructure has a high exciton binding energy (~0.7 eV) and electron mobility rate (~700 cm2/(V·s)). The higher light absorption coefficient, carrier mobility, and exciton energy make the 2D Cs3X2I9/InSe heterostructures suitable for photoluminescent devices. However, the energy band structure based on the Shockley-Queisser limit and type-II arrangement shows that the intrinsic photoelectric conversion efficiency (PCE) of the 2D Cs3X2I9/InSe heterostructure is only about 1.4%, which is not suitable for photovoltaic solar energy. In addition, the modulation and its effect of biaxial strain on the photovoltaic properties of 2D Cs3X2I9/InSe heterostructures are further investigated. The results show that biaxial strain can improve the visible absorption coefficient of 2D Cs3X2I9/InSe heterostructure, but cannot effectively improve its energy band structure, and the PCE only increases to 3.3% at –5% biaxial strain. The above study provides a theoretical basis for designing efficient 2D van der Waals optoelectronic devices in future.
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Keywords:
- 2D heterostructures /
- photoelectric conversion efficiency /
- first-principles calculations /
- strain engineering
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图 1 (a) Cs3Bi2I9/InSe 和(b) Cs3Sb2I9/InSe 的原子结构俯视和侧视图, 其中a和b为晶格矢量, d为 Cs3X2I9层和 InSe 层之间的层间距离
Fig. 1. Top and side views of the atomic structures for the (a) Cs3Bi2I9/InSe heterostructure, and (b) Cs3Sb2I9/InSe heterostructure, where a and b are the lattice vectors and d is the interlayer distance between the Cs3X2I9 and InSe layers.
图 2 (a) Cs3Bi2I9, (b) Cs3Sb2I9和(c) InSe单体结构的HSE06能带结构
Fig. 2. HSE06 band structures of (a) Cs3Bi2I9, (b) Cs3Sb2I9 and (c) InSe monomer structures.
图 3 (a) Cs3Bi2I9/InSe和(b) Cs3Sb2I9/InSe异质结的能带结构; (c) Cs3X2I9/InSe异质结的载流子迁移机制, 其中红色和蓝色分别代表InSe和Cs3X2I9的电子轨道贡献
Fig. 3. Band structures of (a) Cs3Bi2I9/InSe heterostructure and (b) Cs3Sb2I9/InSe heterostructure; (c) carrier migration mechanisms in Cs3X2I9/InSe heterostructures, the red and blue lines represent the electronic orbital contributions for InSe and Cs3X2I9, respectively.
图 4 (a), (b) 二维Cs3Bi2I9/InSe和Cs3Sb2I9/InSe异质结及其各自层在可见光谱中的光吸收系数
Fig. 4. (a), (b) Calculated absorption coefficients of the 2D Cs3Bi2I9/InSe heterostructure and the Cs3Sb2I9/InSe heterostructure and their respective layers in the visible spectrum, respectively.
图 5 (a) Cs3Bi2I9/InSe和(b) Cs3Sb2I9/InSe vdWHs带边的双轴应变
Fig. 5. Biaxial strain on the band edge of (a) Cs3Bi2I9/InSe and (b) Cs3Sb2I9/InSe vdWHs.
图 6 (a) 双轴应变对 (a) Cs3Bi2I9/InSe和(b) Cs3Sb2I9/InSe光吸收系数的影响; (c) Cs3X2I9/InSe结构PCE图
Fig. 6. Biaxial strain on optical absorption coefficients of (a) Cs3Bi2I9/InSe and (b) Cs3Sb2I9/InSe vdWHs; (c) PCE map of intrinsic Cs3X2I9/InSe.
表 2 300 K下的电子和空穴沿x和y方向的有效质量m(m0)、DP常数E1 (eV)、二维弹性模量C2D (N/m)和载流子迁移速率μ2D (cm2·V–1·S–1)
Table 2. Effective masses m(m0), DP E1 (eV), 2D modulus of elasticity C2D (N/m) and carrier mobility μ2D (cm2·V–1·S–1) for electron and hole along and y directions at 300 K.
Carrier type mx my Elx Ely C2D_ x C2D_ y μ2D_ x μ2D_ y Electron Cs3Bi2I9/InSe 0.22 0.23 8.62 8.62 122.96 122.96 472.80 425.55 Cs3Sb2I9/InSe 0.24 0.22 7.13 7.13 125.76 123.22 619.99 692.30 Hole Cs3Bi2I9/InSe 1.16 0.97 6.43 6.43 122.96 122.96 31.39 44.32 Cs3Sb2I9/InSe 1.01 0.75 8.68 8.68 125.76 123.22 23.04 40.94 
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表 1 二维 Cs3X2I9/InSe异质结的晶格常数(a, b)、层间距离(d)、激子结合能(Eb)、带隙(Gap)和晶格失配比(ε)
Table 1. Lattice constants (a, b), interlayer distances (d), exciton binding energy (Eb), band gap (Gap) and lattice mismatch ratio (ε) of 2D Cs3X2I9/InSe heterostructures.
Heterostructure Lattice/Å d /Å Eb /eV Gap/eV ε/% Cs3Bi2I9/InSe a = 8.32 3.71 0.79 1.61 1.89 b = 8.32 Cs3Sb2I9/InSe a = 8.30 3.77 0.73 1.19 1.61 b = 8.30
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