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The next technological step in the exploration of metal‐halide perovskite solar cells is the demonstration of larger‐area device prototypes under outdoor operating conditions. The authors here demonstrate that when slot‐die coating the halide perovskite layers on large areas, ribbing effects may occur but can be prevented by adjusting the precursor ink's rheological properties. For formamidinium lead triiodide (FAPbI3) precursor inks based on 2‐methoxyethanol, the ink viscosity is adjusted by adding acetonitrile (ACN) as a co‐solvent leading to smooth FAPbI3 thin‐films with high quality and layer homogeneity. For an optimized content of 46 vol% of the ACN co‐solvent, a certified steady‐state performance of 22.3% is achieved in p‐i‐n FAPbI3‐perovskite solar cells. Scaling devices to larger areas by making laser series‐interconnected mini‐modules of 12.7 cm2, a power conversion efficiency of 17.1% is demonstrated. A full year of outdoor stability testing with continuous maximum power point tracking on encapsulated devices is performed and it is demonstrated that these devices maintain close to 100% of their initial performance during winter and spring followed by a significant performance decline during warmer summer months. This work highlights the importance of the real‐condition evaluation of larger area device prototypes to validate the technological potential of halide perovskite photovoltaics. [ABSTRACT FROM AUTHOR]

Efficient mixed metal lead‐tin halide perovskites are essential for the development of all‐perovskite tandem solar cells, however they are currently limited by significant short‐circuit current losses despite their near optimal bandgap (≈1.25 eV). Herein, the origin of these losses is investigated, using a combination of voltage dependent photoluminescence (PL) timeseries and various charge extraction measurements. It is demonstrated that the Pb/Sn‐perovskite devices suffer from a reduction in the charge extraction efficiency within the first few seconds of operation, which leads to a loss in current and lower maximum power output. In addition, the emitted PL from the device rises on the exact same timescales due to the accumulation of electronic charges in the active layer. Using transient charge extraction measurements, it is shown that these observations cannot be explained by doping‐induced electronic charges but by the movement of mobile ions toward the perovskite/transport layer interfaces, which inhibits charge extraction due to band flattening. Finally, these findings are generalized to lead‐based perovskites, showing that the loss mechanism is universal. This elucidates the negative role mobile ions play in perovskite solar cells and paves a path toward understanding and mitigating a key loss mechanism. [ABSTRACT FROM AUTHOR]

The development of the simple synthesis schemes of organic semiconductors can have an important contribution to the advancement of related technologies. In particular, one of the fields where the high price of the hole‐transporting materials may become an obstacle toward successful commercialization is perovskite solar cells. Herein, enamine‐based materials that are capable of undergoing cross‐linking due to the presence of two vinyl groups are synthesized. It is shown that new compounds can be thermally polymerized, making the films resistant to organic solvents. This can allow the use of a wet‐coating process for the deposition of the perovskite absorber film, without the need for orthogonal solvents. Cross‐linked films are used in perovskite solar cells, and, upon optimization of the film thickness, the highest power conversion efficiency of 18.1% is demonstrated. [ABSTRACT FROM AUTHOR]

Tandem solar cells are the next step in the photovoltaic (PV) evolution due to their higher power conversion efficiency (PCE) potential than currently dominating, but inherently limited, single‐junction solar cells. With the emergence of metal halide perovskite absorber materials, the fabrication of highly efficient tandem solar cells, at a reasonable cost, can significantly impact the future PV landscape. The perovskite‐based tandem solar cells have already shown that they can convert light more efficiently than their standalone sub‐cells. However, to reach PCEs over 30%, several challenges have to be overcome and the understanding of this fascinating technology has to be broadened. In this review, the main scientific and engineering challenges in the field are presented, alongside a discussion of the current status of three main perovskite tandem technologies: perovskite/silicon, perovskite/CIGS, and perovskite/perovskite tandem solar cells. A summary of the advanced structural, electrical, optical, radiative, and electronic characterization methods as well as simulations being utilized for perovskite‐based tandem solar cells is presented. The main findings are summarized and the strength of the techniques to overcome the challenges and gain deeper knowledge for further performance improvement is assessed. Finally, the PCE potential in different experimental and theoretical limits is compared with an aim to shed light on the path towards overcoming the 30% efficiency threshold for all of the three herein reviewed tandem technologies. [ABSTRACT FROM AUTHOR]

The measurement of the ideality factor (nid) is a popular tool to infer the dominant recombination type in perovskite solar cells (PSC). However, the true meaning of its values is often misinterpreted in complex multilayered devices such as PSC. In this work, the effects of bulk and interface recombination on the nid are investigated experimentally and theoretically. By coupling intensity‐dependent quasi‐Fermi level splitting measurements with drift diffusion simulations of complete devices and partial cell stacks, it is shown that interfacial recombination leads to a lower nid compared to Shockley–Read–Hall (SRH) recombination in the bulk. As such, the strongest recombination channel determines the nid of the complete cell. An analytical approach is used to rationalize that nid values between 1 and 2 can originate exclusively from a single recombination process. By expanding the study over a wide range of the interfacial energy offsets and interfacial recombination velocities, it is shown that an ideality factor of nearly 1 is usually indicative of strong first‐order non‐radiative interface recombination and that it correlates with a lower device performance. It is only when interface recombination is largely suppressed and bulk SRH recombination dominates that a small nid is again desirable. [ABSTRACT FROM AUTHOR]

The effect of sodium doping in NiO as a contact layer for perovskite solar cells is investigated. A combined X‐ray diffraction and X‐ray photoelectron spectroscopy analysis reveals that Na+ mostly segregates as NaOx/NaCl species around NiO crystallites, with the effect of reducing interface capacitance as revealed by impedance spectroscopy. Inspired by this finding, the NiO/perovskite interface in perovskite solar cells is modified via insertion of an ultrathin NaCl interlayer, which increases the NiO work‐function by 0.3 eV. This leads to an increase of power conversion efficiency, approaching 18%, and open‐circuit voltage due to a remarkable suppression of surface recombination, as revealed by photoluminescence analysis and light intensity–dependent electrical measurements. [ABSTRACT FROM AUTHOR]

Today's perovskite solar cells (PSCs) are limited mainly by their open‐circuit voltage (VOC) due to nonradiative recombination. Therefore, a comprehensive understanding of the relevant recombination pathways is needed. Here, intensity‐dependent measurements of the quasi‐Fermi level splitting (QFLS) and of the VOC on the very same devices, including pin‐type PSCs with efficiencies above 20%, are performed. It is found that the QFLS in the perovskite lies significantly below its radiative limit for all intensities but also that the VOC is generally lower than the QFLS, violating one main assumption of the Shockley‐Queisser theory. This has far‐reaching implications for the applicability of some well‐established techniques, which use the VOC as a measure of the carrier densities in the absorber. By performing drift‐diffusion simulations, the intensity dependence of the QFLS, the QFLS‐VOC offset and the ideality factor are consistently explained by trap‐assisted recombination and energetic misalignment at the interfaces. Additionally, it is found that the saturation of the VOC at high intensities is caused by insufficient contact selectivity while heating effects are of minor importance. It is concluded that the analysis of the VOC does not provide reliable conclusions of the recombination pathways and that the knowledge of the QFLS‐VOC relation is of great importance. [ABSTRACT FROM AUTHOR]

In article number 1801892, Steve Albrecht, Vytautas Getautis and co‐workers demonstrate a novel promising concept for the formation of a hole selective monolayer in perovskite solar cells. A low temperature dopant‐free technique makes it suitable for different substrates. [ABSTRACT FROM AUTHOR]

The unprecedented emergence of perovskite‐based solar cells (PSCs) has been accompanied by an intensive search of suitable materials for charge‐selective contacts. For the first time a hole‐transporting self‐assembled monolayer (SAM) as the dopant‐free hole‐selective contact in p–i–n PSCs is used and a power conversion efficiency of up to 17.8% with average fill factor close to 80% and undetectable parasitic absorption is demonstrated. SAM formation is achieved by simply immersing the substrate into a solution of a novel molecule V1036 that binds to the indium tin oxide surface due to its phosphonic anchoring group. The SAM and its modifications are further characterized by Fourier‐transform infrared and vibrational sum‐frequency generation spectroscopy. In addition, photoelectron spectroscopy in air is used for measuring the ionization potential of the studied SAMs. This novel approach is also suitable for achieving a conformal coverage of large‐area and/or textured substrates with minimal material consumption and can potentially be extended to serve as a model system for substrate‐based perovskite nucleation and passivation control. Further gains in efficiency can be expected upon SAM optimization by means of molecular and compositional engineering. A novel concept for the formation of the hole selective layer in efficient perovskite solar cells is presented. Carbazole‐based material is synthesized and used for the formation of a self‐assembled monolayer on top of the indium tin oxide transparent conductive substrate. Power conversion efficiency as high as 17.8% is achieved. [ABSTRACT FROM AUTHOR]