Local halide heterogeneity drives surface wrinkling in mixed-halide wide-bandgap perovskites

Kunal Datta (), Simone C. W. van Laar, Margherita Taddei, Juanita Hidalgo, Tim Kodalle, Guus J. W. Aalbers, Barry Lai, Ruipeng Li, Nobumichi Tamura, Jordi T. W. Frencken, Simon V. Quiroz Monnens, Robert J. E. Westbrook, Daniel J. Graham, Carolin M. Sutter-Fella, Juan-Pablo Correa-Baena, David S. Ginger, Martijn M. Wienk and René A. J. Janssen ()
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Kunal Datta: Eindhoven University of Technology
Simone C. W. van Laar: Eindhoven University of Technology
Margherita Taddei: University of Washington
Juanita Hidalgo: Georgia Institute of Technology
Tim Kodalle: Lawrence Berkeley National Laboratory
Guus J. W. Aalbers: Eindhoven University of Technology
Barry Lai: Argonne National Laboratory
Ruipeng Li: Brookhaven National Laboratory
Nobumichi Tamura: Lawrence Berkeley National Laboratory
Jordi T. W. Frencken: Eindhoven University of Technology
Simon V. Quiroz Monnens: Eindhoven University of Technology
Robert J. E. Westbrook: University of Washington
Daniel J. Graham: University of Washington
Carolin M. Sutter-Fella: Lawrence Berkeley National Laboratory
Juan-Pablo Correa-Baena: Georgia Institute of Technology
David S. Ginger: University of Washington
Martijn M. Wienk: Eindhoven University of Technology
René A. J. Janssen: Eindhoven University of Technology

Nature Communications, 2025, vol. 16, issue 1, 1-13

Abstract: Abstract Compositional heterogeneity in wide-bandgap (1.8 − 2.1 eV) mixed-halide perovskites is a key bottleneck in the processing of high-quality solution-processed thin films and prevents their application in efficient multijunction solar cells. Notably, mixed-cation (formamidinium-methylammonium) wide-bandgap perovskite films are prone to form micrometer-scale wrinkles which can interfere with the smooth surfaces ideal for multijunction devices. Here, we study the formation dynamics of wrinkled mixed-halide perovskite films and its impact on the local composition and optoelectronic properties. We use in situ X-ray scattering during perovskite film formation to show that crystallization of bromide-rich perovskites precedes that of mixed-halide phases in wrinkled films cast using an antisolvent-based process. Using nanoscopic X­-ray fluorescence and hyperspectral photoluminescence imaging, we also demonstrate the formation of iodide- and bromide-rich phases in the wrinkled domains. This intrinsic spatial halide segregation results in an increased local bandgap variation and Urbach energy. Morphological disorder and compositional heterogeneity also aggravate the formation of sub-bandgap electronic defects, reducing photostability and accelerating light-induced segregation of iodide and bromide ions in thin films and solar cells.

Date: 2025
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DOI: 10.1038/s41467-025-57010-6

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