Boosting Carrier Transport in Quasi-2D/3D Perovskite Heterojunction for High-Performance Perovskite/Organic Tandems
Shuaiqing Kang1, Ziyue Wang1, Weijie Chen1（陈炜杰）*, Zhichao Zhang1, Jianlei Cao1, Jialei Zheng1, Xingxing Jiang1, Jiacheng Xu1, Jixiang Yuan1, Juan Zhu1, Haiyang Chen1, Xining Chen1, Yaowen Li1,3,4（李耀文）*, Yongfang Li1,3,5
1Laboratory of Advanced Optoelectronic Materials Suzhou Key Laboratory of Novel Semiconductor-optoelectronics Materials and Devices College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123, China
2College of Physics and Electronics Engineering Hengyang Normal University Hengyang, Hunan 421002, China
3Jiangsu Key Laboratory of Advanced Negative Carbon Technologies Soochow University Suzhou 215123, China
4State and Local Joint Engineering Laboratory for Novel Functional Polymeric Materials Jiangsu Key Laboratory of Advanced Functional Polymer Design and Application College of Chemistry Chemical Engineering and Materials Science Soochow University Suzhou 215123, China
5Beijing National Laboratory for Molecular Sciences CAS Key Laboratory of Organic Solids Institute of Chemistry Chinese Academy of Sciences Beijing 100190, China
Adv. Mater. 2025, 37, 2411027
Abstract: Wide-bandgap (WBG) perovskites are continuously in the limelight owing to their applicability in tandem solar cells. The main bottlenecks of WBG perovskites are interfacial non-radiative recombination and carrier transport loss caused by interfacial defects and large energy-level offsets, which induce additional energy losses when WBG perovskites are stacked with organic solar cells in series because of unbalanced carrier recombination in interconnecting layer (ICL). To solve these issues, 1,3-propanediammonium iodide (PDADI) is incorporated to form Dion–Jacobson -phase quasi-2D perovskites with mixed high-n-values in WBG perovskites. PDADI simultaneously repairs the shallow/deep defects and establishes a Type-II energy-level alignment between quasi-2D/3D and 3D perovskites for rapid carrier extraction. More importantly, the short-chain diammonium cation in quasi-2D perovskite with high n-values results in a short Pb–I inorganic layer spacing, which enhances the interlayer electronic coupling and weakens the quantum-well confinement effect that restricts carrier transport. The suppressed transport loss increases the electron concentration in the ICL for balanced carrier recombination. The 0.0628 and 1.004 cm2 perovskite/organic tandems achieve remarkable efficiencies of 25.92% and 24.63%, respectively. The quasi-2D capping layer can inhibit ion migration, allowing perovskite/organic tandems to show excellent operational stability (T85 > 1000 h).
Article information: //doi.org/10.1002/adma.202411027
