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

Author

Listed:
  • Kunal Datta

    (Eindhoven University of Technology
    Georgia Institute 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
    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
    Pacific Northwest National Laboratory)

  • Martijn M. Wienk

    (Eindhoven University of Technology)

  • René A. J. Janssen

    (Eindhoven University of Technology
    Dutch Institute of Fundamental Energy Research)

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.

Suggested Citation

  • 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 Monnen, 2025. "Local halide heterogeneity drives surface wrinkling in mixed-halide wide-bandgap perovskites," Nature Communications, Nature, vol. 16(1), pages 1-13, December.
  • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-57010-6
    DOI: 10.1038/s41467-025-57010-6
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