4.8 Article

Halide Remixing under Device Operation Imparts Stability on Mixed-Cation Mixed-Halide Perovskite Solar Cells

Journal

ADVANCED MATERIALS
Volume 34, Issue 36, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202202163

Keywords

diffraction; electrostriction; perovskites; photosegregation; photovoltaics

Funding

  1. European Research Council (ERC) under the European Union [756962]
  2. Engineering and Physical Sciences Research Council (EPSRC) [EP/R023980/1, EP/T02030X/1, EP/S030638/1, EP/V027131/1]
  3. EPSRC Departmental Graduate Studentship
  4. Polish Ministry of Science and Higher Education [1603/MOB/V/2017/0]
  5. Royal Society [RGFR1180002]
  6. Taiwan Cambridge Scholarship
  7. Winton Studentship
  8. ICON Studentship from the Lloyd's Register Foundation
  9. European Union [841386]
  10. Leverhulme Early Career Fellowship - Leverhulme Trust [ECF-2019-224]
  11. Isaac Newton Trust
  12. Royal Academy of Engineering
  13. Tata Group [UF150033]
  14. Leverhulme Research Grant [RPG-2021-191]

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Mixed-halide mixed-cation hybrid perovskites are promising for optoelectronic devices due to their high performance and adjustable bandgap. However, their instability caused by ionic migration hinders their further development. This study uses an operando technique to track the structural changes in mixed-halide mixed-cation perovskite solar cells under continuous load and illumination. The results reveal the impact of halide remixing on structural evolution and device instability.
Mixed-halide mixed-cation hybrid perovskites are among the most promising perovskite compositions for application in a variety of optoelectronic devices due to their high performance, low cost, and bandgap-tuning capabilities. Instability pathways such as those driven by ionic migration, however, continue to hinder their further progress. Here, an operando variable-pitch synchrotron grazing-incidence wide-angle X-ray scattering technique is used to track the surface and bulk structural changes in mixed-halide mixed-cation perovskite solar cells under continuous load and illumination. By monitoring the evolution of the material structure, it is demonstrated that halide remixing along the electric field and illumination direction during operation hinders phase segregation and limits device instability. Correlating the evolution with directionality- and depth-dependent analyses, it is proposed that this halide remixing is induced by an electrostrictive effect acting along the substrate out-ofplane direction. However, this stabilizing effect is overwhelmed by competing halide demixing processes in devices exposed to humid air or with poorer starting performance. The findings shed new light on understanding halide de- and re-mixing competitions and their impact on device longevity. These operando techniques allow real-time tracking of the structural evolution in full optoelectronic devices and unveil otherwise inaccessible insights into rapid structural evolution under external stress conditions.

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