Deposition of perovskite films by antisolvent engineering is a highly common method employed in perovskite photovoltaics research. Herein, we report on a general method that allows for the fabrication of highly efficient perovskite solar cells by any antisolvent via manipulation of the antisolvent application rate. Through detailed structural, compositional, and microstructural characterization of perovskite layers fabricated by 14 different antisolvents, we identify two key factors that influence the quality of the perovskite layer: the solubility of the organic precursors in the antisolvent and its miscibility with the host solvent(s) of the perovskite precursor solution, which combine to produce rate-dependent behavior during the antisolvent application step. Leveraging this, we produce devices with power conversion efficiencies (PCEs) that exceed 21% using a wide range of antisolvents. Moreover, we demonstrate that employing the optimal antisolvent application procedure allows for highly efficient solar cells to be fabricated from a broad range of precursor stoichiometries.

Lead halide perovskites are a remarkable class of materials that have emerged over the past decade as being suitable for application in a broad range of devices, such as solar cells, light‐emitting diodes, lasers, transistors, and memory devices. While they are often solution‐processed semiconductors deposited at low temperatures, perovskites exhibit properties one would only expect from highly pure inorganic crystals that are grown at high temperatures. This unique phenomenon has resulted in fast‐paced progress toward record device performance. Unfortunately, the basic science behind the remarkable nature of these materials is still not well understood. This review assesses the current understanding of the photoluminescence properties of metal halide perovskite materials and highlights key areas that require further research. Furthermore, the need to standardize the methods for characterization of PL in order to improve comparability, reliability, and reproducibility of results is emphasized.

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.

Solution-processed quantum dots (QDs) have a high potential for fabricating low cost, flexible and large-scale solar energy harvesting devices. It has recently been demonstrated that hybrid devices employing a single monovalent cation perovskite solution for PbS QD surface passivation exhibit enhanced photovoltaic performance when compared to standard ligand passivation. Herein we demonstrate that the use of a triple cation Cs0.05(MA0.17FA0.83)0.95Pb(I0.9Br0.1)3 perovskite composition for surface passivation of the quantum dots results in highly efficient solar cells, which maintain 96 % of their initial performance after 1200h shelf storage. We confirm perovskite shell formation around the PbS nanocrystals by a range of spectroscopic techniques as well as high-resolution transmission electron microscopy. We find that the triple cation shell results in a favorable energetic alignment to the core of the dot, resulting in reduced recombination due to charge confinement without limiting transport in the active layer. Consequently, photovoltaic devices fabricated via a single-step film deposition reached a maximum AM1.5G power conversion efficiency of 11.3 % surpassing most previous reports of PbS solar cells employing perovskite passivation.

At a current value of 25.5%, perovskites have reached some of the highest power conversion efficiencies of all single-junction solar cell devices. Researchers, however, are questioning their readiness for the commercial market, citing reasons of the toxicity of the lead-based active layer and instability. Closer examination of the life cycle of perovskite solar cells reveals that there are more areas than just these which should be addressed in order to bring an environmentally friendly and sustainable technology to global use. In this review, we discuss these issues. Life cycle analyses show that high temperature processes, heavy use of organic solvents, and extensive use of certain materials can have high up and downstream consequences in terms of emissions, human and ecotoxicity. We further bring attention to the toxicity of the perovskites themselves, where the most direct analyses suggest that the lead cannot be considered totally safe, despite its small quantity and that replacements such as tin may be more toxic in certain scenarios. As a way to reduce the negative environmental impact, we highlight ways in which researchers have used encapsulation and recycling to extend the life of the entire unit and its components and to prevent lead leakage. We hope this review directs researchers toward new strategies to introduce a clean solar technology to the world.

In this work, we examine the effect of microstructure on ion-migrationinduced photoluminescence (PL) quenching in methylammonium lead iodide perovskite films. Thin films were fabricated by two methods: spin-coating, which results in randomly oriented perovskite grains, and zone-casting, which results in aligned grains. As an external bias is applied to these films, migration of ions causes a quenching of the PL signal in the vicinity of the anode. The evolution of this PLquenched zone is less uniform in the spin-coated devices than in the zone-cast ones, suggesting that the relative orientation of the crystal grains plays a significant role in the migration of ions within polycrystalline perovskite. We simulate this effect via a simple Ising model of ionic motion across grains in the perovskite thin film. The results of this simulation align closely with the observed experimental results, further solidifying the correlation between crystal grain orientation and the rate of ionic transport.

The properties of charged point defects in semiconductors such as metal halide perovskites play a critical role in the efficiency and stability of solar cells. Still, the formation and migration enthalpies as well as formation entropies of ionic defects in metal halide perovskites have not yet been determined experimentally. Through impedance spectroscopy, along with a quantification of the ionic defect properties, we demonstrate an approach to obtain ion migration and formation enthalpies as well as formation entropy changes in different metal halide perovskite thin films. We investigate lead-based perovskites that contain different cations (Cs, methylammonium (MA), and formamidinium (FA)) such as MAPbI 3 , CsPbI 3 , and a mixture of all Cs 0.05 (FA 0.83 MA 0.17 ) 0.95 Pb-(I 0.9 Br 0.1 ) 3 . We assign the most dominant, common defect responsible for ion conductivity to iodide vacancy and compare its defect properties in terms of entropy and enthalpy changes in all measured perovskite compositions. Our approach is relevant for ionic conductors in general.