Intermediate-Phase Engineering via Dimethylammonium Cation Additive for Stable Perovskite Solar Cells
David McMeekin a b c, Philippe Holzhey a, Udo Bach a b c, Henry Snaith a
a Department of Physics University of Oxford, Parks Road, United Kingdom
b Department of Chemical Engineering, Monash University, Victoria 3800, Australia
c Monash University, Wellington Road, Clayton, Australia
Materials for Sustainable Development Conference (MATSUS)
Proceedings of Materials for Sustainable Development Conference (MAT-SUS) (NFM22)
#STAPOS - Stability of perovskite and organic solar cells
Barcelona, Spain, 2022 October 24th - 28th
Organizers: Carsten Deibel and Qiong Wang
Contributed talk, David McMeekin, presentation 176
DOI: https://doi.org/10.29363/nanoge.nfm.2022.176
Publication date: 11th July 2022

Achieving long-term stability of perovskite solar cells is arguably the most important challenge required to enable widespread commercialization. Understanding the perovskite crystallization process and its direct impact on device stability is critical to achieve this goal. Surprisingly, we find that intermediate phases that occur during the crystallization process strongly influence the long-term perovskite device stability. The commonly employed “dimethyl formamide/dimethyl sulfoxide” (DMF/DMSO) solvent system preparation method results in poor crystal quality and microstructure of the polycrystalline perovskite films. In this work, we introduce a high-temperature “DMSO-free” processing method that utilizes dimethylammonium chloride (DMACl) as an additive to accurately control the perovskite intermediate precursor-phases. By precisely controlling the 2H to 3C perovskite phase crystallization sequence, we tune the grain size, texturing, orientation (corner-up vs face-up) and crystallinity of the formamidinium (FA)yCs1‑yPb(IxBr1-x)3 perovskite system. A population of encapsulated devices showed significantly improved operational stability, with a median T80 lifetime, for the steady-state PCE, of 1190 hours and a champion device showed a T80 of 1410 hours, under simulated sun light at 65 °C in air, under open‑circuit conditions. Our work introduces an innovative processing method that allows higher overall perovskite device stability, by controlling the intermediate phase domains during the perovskite formation. This work highlights the importance of material quality in order to achieve long-term operational stability of perovskite optoelectronic devices.

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