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Integrated perovskite/organic solar cells (IPOSCs) based on CH3NH3PbI3/PM6:Y6(BTP-4F) are successfully prepared through process innovation and thin film optimization technology. The quality of CH3NH3PbI3/PM6:Y6 mixed films is greatly optimized, and the interlayer ohmic contact is obtained by regulating the additive DIO and annealing treatment. At the same time, the mobility of holes and electrons in the organic layer in the near infrared region are, respectively, 8.3×10–3 cm2/(V·s) and 8.8×10–3 cm2/(V·s), which can match the mobility of holes and electrons in the visible perovskite layer, achieving the carrier transport balance in the microscopic pathway. The device has high short-circuit current density Jsc and high filling factor FF. In addition, by optimizing the mass ratio of polymer non-fullerene system PM6:Y6 to form a film, the density of non-radiation recombination sites and carrier recombination in the film are significantly reduced, making the extraction and transport of electrons and holes more efficient, and providing greater driving force to improve carrier transport. At the same time, a wider depletion region is formed to inhibit carrier recombination and increase the open-circuit voltage Voc. The short-circuit current density of the optimized integrated solar cell increases to 25.88 A/cm2, the open-circuit voltage Voc increases to 1.18 V, the filling factor FF reaches 80%, the optical response expands to 950 nm, the external quantum efficiency reaches 90% in the visible region, and the optimal energy conversion efficiency is as high as 24.42%. This is one of the highest efficiencies reported in IPOSCs. The results show that it is an effective method to enhance the near-infrared light absorption of perovskite solar cells and improve the performance of IPOSCs by combining the materials in visible region and the polymer non-fullerene system in near infrared region and optimizing the device structure. It lays a theoretical foundation for developing high efficiency IPOSCs in the future.
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Keywords:
- integrated perovskite/organic solar cell /
- polymer non-fullerene system /
- carrier transport equilibrium /
- non-radiative recombination
[1] Jeong M, Choi I W, Go E M, Cho Y, Kim M, Lee B, Jeong S, Jo Y, Choi H W, Lee, Bae J H, Kwak S K, Kim D S, Yang C 2020 Science 369 1615
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图 1 聚合物非富勒烯体系PM6:Y6 (BTP-4F)分子结构式 (a) PM6; (b) Y6
Figure 1. Molecular structure formula for polymer non-fullerene system PM6:Y6 (BTP-4F): (a) PM6; (b) Y6.
图 2 聚合物非富勒烯体系PM6:Y6 (BTP-4F)吸收光谱 (a) PM6和Y6纯薄膜; (b) PM6:Y6混合薄膜
Figure 2. Absorption spectra of PM6:Y6 (BTP-4F) in polymer non-fullerene system: (a) PM6 and Y6 pure films; (b) PM6:Y6 mixed films.
图 3 IPOSCs的器件结构与能级搭配图 (a)器件结构; (b)能级排列
Figure 3. Device structure and energy level collocation diagram of IPOSCs: (a) Device structure; (b) energy level alignment.
图 4 质量比不同的IPOSCs PM6:Y6薄膜的AFM和SEM测试 (a)—(c) AFM; (d)—(f) SEM
Figure 4. AFM images and SEM images for PM6:Y6 thin films with different mass ratios in IPOSCs: (a)–(c) AFM; (d)–(f) SEM.
图 5 不同退火温度下IPOSCs CH3NH3PbI3薄膜的AFM和SEM测试 (a)—(c) AFM; (d)—(f) SEM
Figure 5. AFM images and SEM images of CH3NH3PbI3 films of IPOSCs at different annealing temperatures: (a)–(c) AFM; (d)–(f) SEM.
图 6 纯钙钛矿太阳电池、有机光伏电池和IPOSCs的光伏性能、外量子效率、载流子以及阻抗测试 (a)纯钙钛矿太阳电池光伏性能J-V曲线; (b) OSC光伏性能J-V曲线; (c) IPOSCs光伏性能J-V曲线; (d) EQE曲线和积分电流曲线; (e)空穴迁移率; (f)电化学阻抗谱
Figure 6. Photovoltaic performance, external quantum efficiency, carrier and impedance tests of pure perovskite solar cells, organic photovoltaic cells and IPOSCs: (a) J-V curves of photovoltaic performance of pure perovskite solar cells; (b) J-V curves of photovoltaic performance of organic solar cells; (c) performance J-V curves of IPOSCs; (d) EQE curves and integral current curves; (e) hole mobility; (f) electrochemical impedance spectroscopy.
图 7 IPOSCs光伏性能可再现性统计和稳定性测试 (a) 可再现性统计; (b) 稳定性测试
Figure 7. Repeatability statistics and stability test of photovoltaic performance of IPOSCs: (a) Repeatability statistics; (b) stability test.
表 1 IPOSCs光伏性能参数
Table 1. Photovoltaic performance parameters of IPOSCs.
CH3NH3PbI3/
PM6:Y6Voc/V Jsc/(mA·cm–2) FF/% PCE/% 1∶1 1.17 25.02 79 23.12 1∶1.5 1.18 25.88 80 24.42 1∶2 1.16 24.01 78 21.70 
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[1] Jeong M, Choi I W, Go E M, Cho Y, Kim M, Lee B, Jeong S, Jo Y, Choi H W, Lee, Bae J H, Kwak S K, Kim D S, Yang C 2020 Science 369 1615
Google Scholar
[2] Al-Ashouri A, Kohnen E, Li B, Magomedov A, Hempel H, Caprioglio P, Marquez J A, Vilches A B M, Getautis V, Albrecht S 2020 Science 370 1300
Google Scholar
[3] Ono L K, Liu S Z, Qi Y B 2020 Angew. Chem. , Int. Edit. 59 6676
Google Scholar
[4] Jiang Q, Ni Z, Xu G, Lin Y, Rudd P N, Xue R, Li Y, Li Y, Gao Y, Huang J 2020 Adv. Mater. 32 2001581
Google Scholar
[5] Karlsson M, Yi Z, Reichert S, Luo X, Lin W, Zhang Z, Bao C, Friend R, Gao F 2021 Nat. Commun. 12 361
Google Scholar
[6] Dong Q S, Zhu C, Chen M, Jiang C, Guo J Y, Feng Y L, Zhou Y Y 2021 Nat. Commun. 12 9
Google Scholar
[7] Gao C, Yu H, Wang Y, Liu D, Wen T, Zhang L, Ge S, Yu J 2020 Anal. Chem. 92 6822
Google Scholar
[8] Li D Q, Geng F S, Hao T Y, Chen Z 2022 Nano Energy 96 107133
Google Scholar
[9] Gu B K, Du Y, Chen B, Zhao R, Lu H, Xu Q Y, Guo C X 2022 ACS Appl. Mater. Interfaces 14 11264
Google Scholar
[10] Yang X, Li B, Zhang X L, Li S Y 2023 Adv. Mater. DOI: 10.1002/adma.202301604
[11] Lin X F, Cheng P P, Zhang Y W, Tan W Y, Yu D S, Yi G B, Min Y G 2020 Sol. Energy 206 793
Google Scholar
[12] Lin X F, Wang Y Y, Wu J Y, Tang Z L, Lin W J, Nian L, Yi G B 2021 ACS Appl. Energy Mater. 4 5905
Google Scholar
[13] Ma R, Liu T, Luo Z, Guo Q, Xiao Y, Chen Y, Li X, Luo S, Lu X, Zhang M, Li Y, Yan H 2020 Sci. China:Chem. 63 325
Google Scholar
[14] Umeyama T, Igarashi K, Sasada D, Tamai Y, Ishida K, Koganezawa T, Ohtani S, Tanaka K, Ohkita H, Imahori H 2020 Chem. Sci. 11 3250
Google Scholar
[15] Umeyama T, Igarashi K, Sasada D, Ishida K, Tanaka K, Imahori H 2020 ACS Appl. Mater. Interfaces 12 39236
Google Scholar
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