Solar cells incorporating metal‐halide perovskite (MHP) semiconductors are continuing to break efficiency records for solution‐processed solar cell devices. Scaling MHP‐based devices to larger area prototypes requires the development and optimization of scalable process technology and ink formulations that enable reproducible coating results. It is demonstrated that the power conversion efficiency (PCE) of small‐area methylammonium lead iodide (MAPbI3) devices, slot‐die coated from a 2‐methoxy‐ethanol (2‐ME) based ink with dimethyl‐sulfoxide (DMSO) used as an additive depends on the amount of DMSO and age of the ink formulation. When adding 12 mol% of DMSO, small‐area devices of high performance (20.8%) are achieved. The effect of DMSO content and age on the thin film morphology and device performance through in situ X‐ray diffraction and small‐angle X‐ray scattering experiments is rationalized. Adding a limited amount of DMSO prevents the formation of a crystalline intermediate phase related to MAPbI3 and 2‐ME (MAPbI3‐2‐ME) and induces the formation of the MAPbI3 perovskite phase. Higher DMSO content leads to the precipitation of the (DMSO)2MA2Pb3I8 intermediate phase that negatively affects the thin‐film morphology. These results demonstrate that rational insights into the ink composition and process control are critical to enable reproducible large‐scale manufacturing of MHP‐based devices for commercial applications.

Antimony nanoparticles grown on highly oriented pyrolytic graphite and molybdenum disulfide were used as a model system to investigate the contact-area dependence of frictional forces. This system allows one to accurately determine both the interface structure and the effective contact area. Controlled translation of the antimony nanoparticles ͑areas between 10 000 and 110 000 nm 2 ͒ was induced by the action of the oscillating tip in a dynamic force microscope. During manipulation, the power dissipated due to tip-sample interactions was recorded. We found that the threshold value of the power dissipation needed for translation depends linearly on the contact area between the antimony particles and the substrate. Assuming a linear relationship between dissipated power and frictional forces implies a direct proportionality between friction and contact area. Particles about 10 000 nm 2 in size, however, were found to show dissipation close to zero. To explain the observed behavior, we suggest that structural lubricity might be the reason for the low dissipation in the small particles, while elastic multistabilities might dominate energy dissipation in the larger particles.

Through the optimization of the perovskite precursor composition and interfaces to selective contacts, we achieved a p-i-n-type perovskite solar cell (PSC) with a 22.3% power conversion efficiency (PCE). This is a new performance record for a PSC with an absorber bandgap of 1.63 eV. We demonstrate that the high device performance originates from a synergy between (1) an improved perovskite absorber quality when introducing formamidinium chloride (FACl) as an additive in the “triple cation” Cs0.05FA0.79MA0.16PbBr0.51I2.49 (Cs-MAFA) perovskite precursor ink, (2) an increased open-circuit voltage, V OC, due to reduced recombination losses when using a lithium fluoride (LiF) interfacial buffer layer, and (3) high-quality hole-selective contacts with a self-assembled monolayer (SAM) of [2-(9H-carbazol-9-yl)­ethyl]­phosphonic acid (2PACz) on ITO electrodes. While all devices exhibit a high performance after fabrication, as determined from current–density voltage, J–V, measurements, substantial differences in device performance become apparent when considering longer-term stability data. A reduced long-term stability of devices with the introduction of a LiF interlayer is compensated for by using FACl as an additive in the metal-halide perovskite thin-film deposition. Optimized devices maintained about 80% of the initial average PCE during maximum power point (MPP) tracking for >700 h. We scaled the optimized device architecture to larger areas and achieved fully laser patterned series-interconnected mini-modules with a PCE of 19.4% for a 2.2 cm2 active area. A robust device architecture and reproducible deposition methods are fundamental for high performance and stable large-area single junction and tandem modules based on PSCs.

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The spontaneous formation of complex interfacial patterns from thermally deposited Sb 4 clusters on HOPG is controlled by the deposition conditions (i.e., coverage and deposition rate) at constant temperature (300 K) under ultrahigh vacuum conditions. Two main driving forces for the pattern formation in this system have been identified. Initially, the crystallization of compact nanoparticles with spherical shape at a maximum diameter of 120 nm drives the system toward irregular, fingerlike shapes. Second, the ramification of these fingerlike nanoparticles is governed by the deposition rate, as the increase of the deposition rate allows the nanoparticle shape to be continuously tuned from fingerlike to further ramified and eventually fractal forms. On the basis of electron microscopy and atomic force microscopy measurements, these phenomena are quantified with a focus on fractal dimension, particle perimeter, and size of the side branches (tip width). † Part of the special issue "Gerhard Ertl Festschrift".