A Dimethylammonium-Induced Intermediate Phase Approach Towards Stable Formamidinium-Caesium-based Perovskite Solar Cells
David McMeekin a b c, Philippe Holzhey a, ‪Sebastian O. Fürer b c, Steve P. Harvey d, Laura T. Schelhas e, James M. Ball a, Suhas Mahesh a, Nicholas Hawkins f, Jianfeng Lu b c, Fritz Vollrath f, Michael B. Johnston a, Joseph J. Berry d, Udo Bach b c, Henry J. Snaith a
a Clarendon Laboratory, Department of Physics, University of Oxford, Parks Road, Oxford, United Kingdom
b Department of Chemical Engineering, Monash University, Victoria 3800, Australia
c ARC Centre of Excellence for Exciton Science, Monash University, Victoria, Australia
d Material Science Center, National Renewable Energy Laboratory, Golden, CO 80401, USA, Denver West Parkway, 15013, Golden, United States
e Applied Energy Programs, SLAC National Accelerator Laboratory, Sand Hill Road, 2575, Menlo Park, United States
f Department of Zoology, University of Oxford, 11a Mansfield Rd, Oxford, United Kingdom
g Applied Energy Programs, SLAC National Accelerator Laboratory, Sand Hill Road, 2575, Menlo Park, United States
International Conference on Hybrid and Organic Photovoltaics
Proceedings of 13th Conference on Hybrid and Organic Photovoltaics (HOPV21)
Online, Spain, 2021 May 24th - 28th
Organizers: Marina Freitag, Feng Gao and Sam Stranks
Invited Speaker Session, David McMeekin, presentation 085
Publication date: 11th May 2021

Achieving long-term stability of perovskite solar cells is arguably the most important challenge required to enable widespread commercialization. Understanding the impact of the perovskite material quality on device stability is critical to overcoming this hurdle. Surprisingly, we found that the fabrication methods had significant impact on the overall perovskite stability. The commonly employed “DMF/DMSO” solvent system preparation method resulted in poor crystal quality and microstructure, which ultimately lead to an inferior material stability compared the “DMF/acid” or “DMF/DMA” processing method, proposed in this work. These fabrication methods exhibited a high degree of texturing and crystallinity. Furthermore, we observe residual DMSO in the perovskite film, which could adversely affect the stability of the material. In this work, we introduce a high temperature “DMSO-free” processing method that utilizes DMACl to accurately control the perovskite precursor phases. By precisely controlling the 2H to 3C crystallization sequence rate, we can tune the size, texturing, orientation (corner-up vs face-up) and crystallinity of the crystal grain to extend the long‑term operational lifetime of the (FA,Cs)Pb(Br,I)3 perovskite system. We investigated the impact of these various crystal quality film on the stability of the perovskite by decoupling the main degradation mechanisms (humidity, heat and light). A population of encapsulated devices showed a t80 lifetime, for the stabilized PCE, of 1190 h as median value and a champion device showing a t80 of 1410 h, under simulated sun light at 65 °C in air, under open‑circuit conditions, in contrast to a median value of t80 = 1040 h and a champion t80 = 780 h for conventional DMF/DMSO devices. Our work introduces an innovative processing method that allows higher overall perovskite device stability, by controlling the intermediate phases domains during the perovskite formation. This work highlights the importance of material quality in order to achieve long-term operational stability of perovskite solar cells.

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