Reproducibility issues of perovskite materials and devices stem from their extreme sensitivity to fractional, quite possibly unintentional, deviations in the precursor solution stoichiometry.

photovoltaic technology, where lifetimes greater than 25 years are required. [2] Although the issue of device stability has attracted increased attention of the photovoltaic research community in the last two years, reports that systematically study the fundamental causes (e.g., heat, electrical stress, humidity, oxygen, (UV) light, chemical precursors, processing conditions, influence of film quality and morphology) and mechanisms limiting the material and device stability remain scarce. [2][3][4][5] While the degradation of methylammonium lead iodide (MAPbI 3 ) in humid air has been studied experimentally as well as theoretically and was long thought to be the main factor for material degradation in ambient environment, [6][7][8][9][10][11][12][13][14][15] studies exploring the influence of oxygen and light on the solar cell performance have only recently been reported. [16][17][18][19][20] It has been shown that photoexcited electrons in the perovskite layer can form superoxide (O 2 − ) via electron transfer to molecular oxygen, which through deprotonation of the methylammonium cation in turn results in irreversible material degradation. The severity of the degradation has been linked to the efficiency of electron extraction via the electron extracting layer (EEL): devices employing a compact-TiO 2 /mesoporous Al 2 O 3 or compact-TiO 2 as EELs degraded in dry air on a timescale of less than 1 h, while with the use of a mesoporous TiO 2 layer, an EEL which results in faster electron extraction, the lifetimes were significantly increased. However, in these reports only the degradation of complete photovoltaic device was reported, with limited information on the degradation of the perovskite active layer itself and the impact of its microstructure was not identified.In this work, we systematically study the degradation of MAPbI 3 films under precisely controlled exposure to various oxygen levels (0-20%) under simulated sunlight in order to shed light on the progression of perovskite degradation under these conditions. We investigate two types of perovskite layers that are formed using different fabrication methods. The two recipes allow us to include the effect of layer microstructure on the dynamics of oxygen-induced degradation. We characterize the electronic, optical, compositional, and structural properties of the degraded perovskite films and correlate these results This paper investigates the impact of microstructure on the degradation rate of methylammonium lead triiodide (MAPbI 3 ) perovskite films upon exposure to light and oxygen. By comparing the oxygen induced degradation of perovskite films of different microstructure-fabricated using either a lead acetate trihydrate precursor or a solvent engineering technique-it is demonstrated that films with larger and more uniform grains and better electronic quality show a significantly reduced degradation compared to films with smaller, more irregular grains. The effect of degradation on the optical, compositional, and microstructural properties of the perovsk...

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In article number https://doi.org/10.1002/aenm.201700977, Yana Vaynzof and co‐workers investigate how the MAPbI3 perovskite layer microstructure is affecting its stability upon exposure to oxygen and light. The authors show that the degradation process is initiated at the grain boundaries, demonstrating that devices whose active layer consists of larger, more uniform grains exhibit enhanced photovoltaic stability.