Cation interdiffusion control for 2D/3D heterostructure formation and stabilization in inorganic perovskite solar modules

Cheng Liu, Yi Yang, Jared D. Fletcher, Ao Liu, Isaiah W. Gilley, Charles Bruce Musgrave, Zaiwei Wang, Huihui Zhu, Hao Chen, Robert P. Reynolds, Bin Ding, Yong Ding, Xianfu Zhang, Raminta Skackauskaite, Haoyue Wan, Lewei Zeng, Abdulaziz S. R. Bati, Naoyuki Shibayama, Vytautas Getautis, Bin Chen, Kasparas Rakstys (), Paul J. Dyson (), Mercouri G. Kanatzidis (), Edward H. Sargent () and Mohammad K. Nazeeruddin ()
Additional contact information
Cheng Liu: Northwestern University
Yi Yang: Northwestern University
Jared D. Fletcher: Northwestern University
Ao Liu: Northwestern University
Isaiah W. Gilley: Northwestern University
Charles Bruce Musgrave: Northwestern University
Zaiwei Wang: University of Toronto
Huihui Zhu: Northwestern University
Hao Chen: Northwestern University
Robert P. Reynolds: Northwestern University
Bin Ding: École Polytechnique Fédérale de Lausanne (EPFL)
Yong Ding: École Polytechnique Fédérale de Lausanne (EPFL)
Xianfu Zhang: Northwestern University
Raminta Skackauskaite: Kaunas University of Technology
Haoyue Wan: Northwestern University
Lewei Zeng: University of Toronto
Abdulaziz S. R. Bati: Northwestern University
Naoyuki Shibayama: Toin University of Yokohama
Vytautas Getautis: Kaunas University of Technology
Bin Chen: Northwestern University
Kasparas Rakstys: Kaunas University of Technology
Paul J. Dyson: École Polytechnique Fédérale de Lausanne (EPFL)
Mercouri G. Kanatzidis: Northwestern University
Edward H. Sargent: Northwestern University
Mohammad K. Nazeeruddin: École Polytechnique Fédérale de Lausanne (EPFL)

Nature Energy, 2025, vol. 10, issue 8, 981-990

Abstract: Abstract Inorganic perovskite solar cells could benefit from surface passivation using 2D/3D perovskite heterostructures. However, conventional spacer cations fail to exchange with the tightly bonded Cs cation in the inorganic perovskite to form 2D layers atop; or, when they do enable formation of a 2D layer, they migrate under heat, degrading device performance. Here we investigate the mechanisms behind 2D/3D heterostructure formation and stabilization. We find that 2D/3D heterostructure formation is driven by interactions between ammonium groups and [PbI6]4− octahedra. We thus incorporate electron-withdrawing fluorine to enhance inorganic–organic cation interdiffusion and promote heterostructure formation. We note that stability relies on interactions between the entire spacer cations and [PbI6]4− octahedra. We therefore introduce anchoring groups that double cation desorption energies, preventing cation migration at elevated temperatures. CsPbI3/(perfluoro-1,4-phenylene)dimethanammonium lead iodide heterostructures enable an efficiency of 21.6% and a maximum power point operating stability at 85 °C of 950 h. We demonstrate 16-cm2 modules with an efficiency of 19.8%.

Date: 2025
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DOI: 10.1038/s41560-025-01817-6

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