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...

Advancing inverted (p-i-n) perovskite solar cells (PSCs) is key to further enhance the power conversion efficiency (PCE) and stability of flexible and perovskite-based tandem photovoltaics. Yet, the presence of defects...

Wide-bandgap perovskite solar cells (PSCs) with optimal bandgap (E g ) and high power conversion efficiency (PCE) are key to high-performance perovskite-based tandem photovoltaics. A 2D/3D perovskite heterostructure passivation is employed for double-cation wide-bandgap PSCs with engineered bandgap (1.65 eV ≤ E g ≤ 1.85 eV), which results in improved stabilized PCEs and a strong enhancement in open-circuit voltages of around 45 mV compared to reference devices for all investigated bandgaps. Making use of this strategy, semitransparent PSCs with engineered bandgap are developed, which show stabilized PCEs of up to 25.7% and 25.0% in fourterminal perovskite/c-Si and perovskite/CIGS tandem solar cells, respectively. Moreover, comparable tandem PCEs are observed for a broad range of perovskite bandgaps. For the first time, the robustness of the four-terminal tandem configuration with respect to variations in the perovskite bandgap for two state-of-the-art bottom solar cells is experimentally validated.

Large datasets are now ubiquitous as technology enables higher-throughput experiments, but rarely can a research field truly benefit from the research data generated due to inconsistent formatting, undocumented storage or improper dissemination. Here we extract all the meaningful device data from peer-reviewed papers on metal-halide perovskite solar cells published so far and make them available in a database. We collect data from over 42,400 photovoltaic devices with up to 100 parameters per device. We then develop open-source and accessible procedures to analyse the data, providing examples of insights that can be gleaned from the analysis of a large dataset. The database, graphics and analysis tools are made available to the community and will continue to evolve as an open-source initiative. This approach of extensively capturing the progress of an entire field, including sorting, interactive exploration and graphical representation of the data, will be applicable to many fields in materials science, engineering and biosciences.

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Perovskite-based solar cells are promising because of their rapidly improving efficiencies but suffer from instability issues. Recently, it has been claimed that one of the key contributors to the instability of perovskite solar cells is ion migration-induced electrode degradation, which can be avoided by incorporating inorganic hole-blocking layers (HBLs) in the device architecture. In this work, we investigate the operational environmental stability of methylammonium lead iodide perovskite solar cells that contain either an inorganic or organic HBL, with only the former effectively blocking ions from migrating to the metal electrode. This is confirmed by X-ray photoemission spectroscopy measured on the electrodes of degraded devices, where only electrodes of devices with an organic HBL show a significant iodine signal. Despite this, we show that when these devices are degraded under realistic operational conditions (i.e., constant illumination in a variety of atmospheric conditions), both types of devices exhibit nearly identical degradation behavior. These results demonstrate that contrary to prior suggestions, ion-induced electrode degradation is not the dominant factor in perovskite environmental instability under operational conditions.

This work investigates the effect of energetically shallow and deep surface defects in MAPbI3 films on the evolution of their photoluminescence properties upon exposure to ambient environment.