DOI: https://doi.org/10.29363/nanoge.hpatom.2022.017
Publication date: 30th October 2021
Hybrid halide perovskites have drawn significant attention due to their outstanding photovoltaic capabilities. However, these materials exhibit poor environmental stability with respect to moisture, light, and temperature, which limits the performance of solar cells. We demonstrate moisture-induced degradation in the state-of-the-art triple cation mixed halide (Cs0.05(MA0.17FA0.83)0.95Pb(Br0.17I0.83)3). Exposing this material at 85% relative humidity (RH) leads to degradation via two competitive pathways: (i) irreversible phase-segregation to form CsPb2Br5 and a cesium-poor/iodide rich Cs0.05-x(MA0.17FA0.83)0.95Pb(Br0.17-2yI0.83+2y)3 phase and (ii) PbI2 formation via dissolution/recrystallization mechanism. Multi-technique approach utilized in this work facilitates the understanding of this process as aged material consists of crystalline CsPb2Br5 and PbI2 phases that can be characterized using in situ X-ray diffraction and in situ live liquid cell transmission electron microscopy, whereas insights into the local environments of organic as well as inorganic cations are provided by ex-situ 1D/2D solid-state NMR spectroscopy of protons and 133Cs spin-7/2 isotope. Optical spectroscopic techniques, such as photoluminescence (PL) and fluorescence lifetime imaging microscopy, further elucidate the heterogeneities in terms of morphology, PL intensities, and PL lifetimes upon exposure to moisture (85% RH). These results provide new insights into the degradation pathways of this complex yet high-performing composition.
This work has received financial support from Région Hauts-de-France, FEDER, and Electricité de France
(EDF) through PEROVSTAB program. We thank the electronic microscopy platform of UPJV for access to SEM and TEM microscopes. Dr. Anurag Krishna (LRCS and EPFL), Dr. Sebastien Gottis (LRCS), and Dr. Jean-Noel Chotard (LRCS) is acknowledged for fruitful discussions. M.A.A.K and F.S. gratefully acknowledge the financial support from the IR-RMN-THC FR-3050 CNRS France for conducting solid- state NMR measurements. P.R. and G.N.M.R. acknowledge the financial support from University of Lille and région Hauts-de-France. F.S. acknowledges “IMPRESSIVE” project which received funding from the European Union’s Horizon2020 research and innovation program under grant agreement number N° 826013.