Thermally-induced drift of A-site cations at solid-solid interface in physically paired lead halide perovskites

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2022
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Cuzzupè, Daniele T.
Ünlü, Feray
Lê, Khan
Bernhardt, Robin
Wilhelm, Michael
Grosch, Matthias
Weißing, Rene
van Loosdrecht, Paul H. M.
Mathur, Sanjay
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Scientific reports. Springer Nature. 2022, 12(1), 10241. eISSN 2045-2322. Available under: doi: 10.1038/s41598-022-14452-y
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The promise of hybrid organic-inorganic halide perovskite solar cells rests on their exceptional power conversion efficiency routinely exceeding 25% in laboratory scale devices. While the migration of halide ions in perovskite thin films has been extensively investigated, the understanding of cation diffusion remains elusive. In this study, a thermal migration of A‑site cations at the solid-solid interface, formed by two physically paired MAPbI3 and FAPbI3 perovskite thin films casted on FTO, is demonstrated through continuous annealing at comparably low temperature (100 °C). Diffusion of methylammonium (CH3NH3+, MA+) cations into the low‑symmetry yellow δ‑FAPbI3 phase triggers a transition from the yellow (δ) to black (α) phase evident in the distinctive color change and verified by shifts in absorption bands and X‑ray diffraction patterns. Intermixing of the A‑site cations MA+ and FA+ (CH(NH2)2+) occurred for both systems, α‑MAPbI3/δ‑FAPbI3 and α‑MAPbI3/α‑FAPbI3. The structural and compositional changes in both cases support a thermally activated ion drift unambiguously demonstrated through changes in the absorption and X-ray photoelectron spectra. Moreover, the physical contact annealing (PCA) leads to healing of defects and pinholes in α‑MAPbI3 thin films, which was correlated to longer recombination lifetimes in mixed MAxFA1-xPbI3 thin films obtained after PCA and probed by ultrafast transient absorption spectroscopy.

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ISO 690CUZZUPÈ, Daniele T., Feray ÜNLÜ, Khan LÊ, Robin BERNHARDT, Michael WILHELM, Matthias GROSCH, Rene WEISSING, Thomas FISCHER, Paul H. M. VAN LOOSDRECHT, Sanjay MATHUR, 2022. Thermally-induced drift of A-site cations at solid-solid interface in physically paired lead halide perovskites. In: Scientific reports. Springer Nature. 2022, 12(1), 10241. eISSN 2045-2322. Available under: doi: 10.1038/s41598-022-14452-y
BibTex
@article{Cuzzupe2022-06-17Therm-58047,
  year={2022},
  doi={10.1038/s41598-022-14452-y},
  title={Thermally-induced drift of A-site cations at solid-solid interface in physically paired lead halide perovskites},
  number={1},
  volume={12},
  journal={Scientific reports},
  author={Cuzzupè, Daniele T. and Ünlü, Feray and Lê, Khan and Bernhardt, Robin and Wilhelm, Michael and Grosch, Matthias and Weißing, Rene and Fischer, Thomas and van Loosdrecht, Paul  H. M. and Mathur, Sanjay},
  note={Article Number: 10241}
}
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