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双钙钛矿太阳能电池以其低成本、高性能、环境友好、稳定性强而备受关注. 本研究使用Silvaco TCAD分析了Cs2AgBi0.75Sb0.25Br6太阳能电池的钙钛矿层厚度、能带偏移、金属电极功函数、传输层厚度及掺杂浓度与器件效率的关系, 以提升器件性能. 基于空穴传输层为Spiro-OMeTAD, 电子传输层为ZnO的器件进行初始研究, 其显示出12.66%的光电转换效率. 结果表明, 当钙钛矿层厚度大于500 nm时, 效率趋于饱和. 最佳导带偏移量为0—+0.5 eV, 最佳价带偏移量为–0.1—+0.2 eV. 在改变器件的电子传输层为ZnOS, 空穴传输层分别为MoO3, Cu2O和CuSCN的情况下, 优化其厚度和掺杂浓度, 最终空穴传输层为Cu2O的双钙钛矿太阳能电池理论光电转换效率达22.85%, 比目前报道的理论效率值相对提升了25.6%. 此外, 当金属电极功函数小于–4.9 eV时易实现最佳效率. 本工作为开发高性能无铅钙钛矿太阳能电池提供了理论指导.Double perovskite solar cells have attracted much attention due to their low cost, high performance, environmental friendliness, and strong stability. In this study, the effect of thickness of perovskite layer, band offset, metal electrode work function, the thickness and doping concentration of the transport layer on the efficiency of Cs2AgBi0.75Sb0.25Br6 solar cells are analyzed by using Silvaco TCAD to improve device performance. This preliminary study of device based on Spiro-OMeTAD as hole transport layer (HTL) and ZnO as electron transport layer (ETL) shows that the photovoltaic conversion efficiency (PCE) is 12.66%. The results show that the efficiency gradually saturates when the thickness of the perovskite layer is greater than 500 nm. The optimal conduction band offset (CBO) ranges from 0 eV to +0.5 eV and the optimal valence band offset (VBO) from –0.1 eV to +0.2 eV. After changing the device's ETL into ZnOS and HTLs into MoO3, Cu2O and CuSCN, respectively, and optimizing their thickness values and doping concentrations, the final theoretical photovoltaic conversion efficiency of the double perovskite solar cell with an HTL of Cu2O can reach 22.85%, which is increased by 25.6% compared with the currently reported theoretical efficiency value. Moreover, the optimal efficiency is achieved when the metal electrode work function is less than –4.9 eV. This work will help find suitable materials for the transport layer and provide guidance for developing the high-performance and lead-free perovskite solar cells.
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Keywords:
- double perovskite solar cell /
- photoelectric conversion efficiency /
- band offset /
- electrode work function
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图 1 模拟双钙钛矿太阳能电池的二维结构图
Fig. 1. Two-dimensional structure diagram of simulated double perovskite solar cell.
图 2 器件性能随Cs2AgBi0.75Sb0.25Br6厚度的变化
Fig. 2. Variation of device performance with different thickness of Cs2AgBi0.75Sb0.25Br6.
图 3 导带偏移量为(a)负值与(b)正值时的能带排列图; 价带偏移量为(c)负值与(d)正值时的能带排列图
Fig. 3. Energy band alignment diagram with (a) negative and (b) positive CBO; energy band alignment diagram with (c) negative and (d) positive VBO.
图 4 不同(a)导带偏移量和(b)价带偏移量下Cs2AgBi0.75Sb0.25Br6太阳能电池器件性能变化
Fig. 4. Variation of device performance of Cs2AgBi0.75Sb0.25Br6 solar cells with different (a) CBOs and (b) VBOs.
图 5 Cs2AgBi0.75Sb0.25Br6太阳能电池的不同 (a)负值导带偏移量, (b)正值导带偏移量, (d)负值价带偏移量, (e)正值价带偏移量的能带图; 不同(c)负值导带偏移量和(f)负值价带偏移量下界面缺陷层的载流子复合速率
Fig. 5. Energy band diagrams of Cs2AgBi0.75Sb0.25Br6 solar cells with different (a) negative CBOs, (b) positive CBOs, (d) negative VBOs, (e) positive VBOs; carrier recombination rate in interfacial defect layers with different (c) negative CBOs and (f) negative VBOs.
图 6 不同 (a) ZnOS厚度, (b) HTL厚度, (c) ZnOS掺杂浓度, (d) HTL掺杂浓度下Cs2AgBi0.75Sb0.25Br6太阳能电池的器件性能
Fig. 6. Device performance of Cs2AgBi0.75Sb0.25Br6 solar cell with different (a) thickness of ZnOS, (b) thickness of HTL, (c) doping concentration of ZnOS, (d) doping concentration of HTL.
图 7 不同HTL的Cs2AgBi0.75Sb0.25Br6太阳能电池的(a) J-V曲线图和输出参数, (b)能带图
Fig. 7. (a) J-V curves and output parameters, (b) energy band diagrams of Cs2AgBi0.75Sb0.25Br6 solar cells with different HTL.
图 8 Cs2AgBi0.75Sb0.25Br6太阳能电池的能带图随Cu2O掺杂浓度变化
Fig. 8. Variation of energy band diagrams of Cs2AgBi0.75Sb0.25Br6 solar cells with the doping concentration of Cu2O.
图 9 不同功函数对Cs2AgBi0.75Sb0.25Br6太阳能电池性能的影响
Fig. 9. Effect of different work functions on the performance of Cs2AgBi0.75Sb0.25Br6 solar cells.
图 10 (a)不同金属功函数下的器件能带图; 钙钛矿层的(b)电子浓度和(c)空穴浓度随不同金属功函数的变化
Fig. 10. (a) Device energy band diagrams with different metal work functions; variation of (b) electron concentration and (c) hole concentration in perovskite layer with different metal work functions.
表 1 Cs2AgBi0.75Sb0.25Br6太阳能电池各层材料的参数
Table 1. Parameters of each layer material of Cs2AgBi0.75Sb0.25Br6 solar cell.
Parameter ZnO ZnOS Cs2AgBi0.75Sb0.25Br6 Spiro-OMeTAD MoO3 Cu2O CuSCN Permittivity, εr 9[29] 9[18] 6.5[30,31] 3[32] 12.5[33] 7.1[34] 10[35] Band gap/eV 3.3[36] 2.83[37] 1.8[8] 3[38] 3[39] 2.17[40] 3.4[41] Affinity/eV 4[42] 3.6[37] 3.58[43] 2.45[32] 2.5[44] 3.2[45] 1.9[46] NC/cm–3 3.7×1018 2.2×1018 2.2×1018 2.2×1018 2.2×1018 2.02×1017 2.2×1018 NV/cm–3 1.8×1019 1.8×1019 1.8×1019 1.8×1019 1.8×1019 1.1×1019 1.8×1019 ND/cm–3 1×1017 1×1017 1.0×1013 0 0 0 0 NA/cm–3 0 0 1.0×1017 1×1018 1×1018 1×1019 1×1019 μn/(cm2·V–1·S–1) 100 100 2 2×10–4 25 200 100 μp/(cm2·V–1·S–1) 25 25 2 2×10–4 100 80 25 
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表 2 优化的器件光伏性能参数及参考
Table 2. Optimized device photovoltaic performance parameters and references.
Thickness/nm Doping
concentration/cm–3VOC/V JSC/(mA·cm–2) PCE/% FF/% This work ZnOS/Cs2AgBi0.75Sb0.25Br6/Cu2O:
70/400/350ETL/HTL: 2×1018/9×1021 1.36 14.12 16.87 88.04 After thickness optimization ZnOS/Cs2AgBi0.75Sb0.25Br6/Cu2O:
30/500/280ETL/HTL: 2×1018/9×1021 1.36 15.70 18.56 87.24 After ND(ZnOS) optimization ZnOS/Cs2AgBi0.75Sb0.25Br6/Cu2O:
30/500/280ETL/HTL: 1×1020/9×1021 1.35 15.70 18.62 87.37 After NA(Cu2O) optimization ZnOS/Cs2AgBi0.75Sb0.25Br6/Cu2O:
30/500/280ETL/HTL: 1×1020/1×1017 1.35 19.49 22.85 86.76 Ref.[14] ZnOS/Cs2AgBi0.75Sb0.25Br6/Cu2O:
70/400/350ETL/HTL: 2×1018/9×1021 1.39 16.04 18.18 78.34 Other Ref.[58] ZnO/Cs2AgBi0.75Sb0.25Br6/NiO:
70/400/350ETL/HTL: 5×1017/3×1018 1.23 15.57 17.13 89.39 Other Ref.[13] NiO/Cs2AgBi0.75Sb0.25Br6/PCBM/
SnO2: 40/500/40/6ETL/HTL: 1×1015/5×1017 1.14 14.9 10.01 58.70
下载: 导出CSV
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