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Indium-Based Octahedra Coordinating Pb-I Termini for Stable Perovskites
Yehui Wen1,2, Yueqi Shen3, Xingtao Wang4
1State Key Laboratory of Silicon and Advanced Semiconductor Materials and School of Materials Science and Engineering, Zhejiang University, Hangzhou, Zhejiang, P. R. China.
Abstract:
Halide perovskite degradation initiates at surfaces/interfaces, where defect accumulation disrupts octahedral connectivity and triggers structural collapse. Herein, we design an indium-based octahedral motifs, i.e., (PMA)4InCl7 (PIC) (PMA=phenylmethylammonium) featuring disordered octahedra and (PMA)4NaInCl8 (PNIC) with ordered octahedral frameworks, as robust coordination agent to bind Pb-I termini at the surface/interface. Distinct from the isolated cluster of PIC, PNIC forms a coherent inorganic framework at Pb-I termini, enabling coherent interfacial coupling with the 3D perovskite via octahedral-level coupling between In(Na)-Cl and Pb-I units. This rigid octahedral coupling immobilizes formamidinium cations and Pb-I octahedra at the surface/interface, suppressing structural freedom. Moreover, this coupling facilitates the relaxation of interfacial structural imperfections while simultaneously establishing favorable band alignment, together governing enhanced carrier transport dynamics. As a result, the resulting perovskite solar cells deliver an efficiency of 27.29% (certified 26.84%), with the minimodules reaching 24% (certified 23.54%). Moreover, these devices demonstrate significant operational stability, retaining over 98% of their initial efficiency after 3,000 h of maximum power point tracking.
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