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The main advantages of the organic–inorganic halide perovskite solar cell technology are high efficiencies achieved after short development time in combination with rather simple solution-based processing. In this paper, we address remaining challenges by presenting a low-temperature two-step hybrid evaporation-spincoating method that combines high reproducibility with easy fabrication and high stabilized efficiencies, which is compatible with the processing of pervoskite silicon tandem solar cells and avoids using hazardous solvents such as dimethylformamide and dimethylsulfoxide. Lead iodide (PbI2) is thermally evaporated and subsequently converted into a compact crystalline perovskite layer by methylammonium iodide spincoating. Moreover, the role of the interface passivation between perovskite absorber and electron transport layer on crystallization and optoelectronic properties of the perovskite absorber is investigated within a systematic thickness and concentration variation of [6, 6]-phenyl-C61-butyric acid methyl ester passivation layer and by analyzing charge extraction with spatial and time resolved photoluminescence measurements. With an optimized charge extraction, 18.2% stabilized efficiency under one sun illumination is achieved. This is the highest value reported so far for the single junction perovskite solar cells made by a two-step hybrid evaporation-spincoating method.

Electroplated copper contacts on small-area single-junction perovskite solar cells (PSCs) using an atomic layer deposited (ALD) Al2O3 masking layer on ITO are demonstrated for the first time. The photoconversion efficiency of ≈11% after manufacturing the Cu contacts confirms that PSCs can survive the wet-chemical plating process. From the successful realization of plated contact fingers, the creation of an electrical contact between the Cu electrode and the ITO on the FA0.75Cs0.25Pb(I0.8Br0.2)3 perovskite absorber is inferred. Furthermore, scanning electron microscopy (SEM) with energy-dispersive X-ray (EDX) analysis shows the formation of a compact interface between ITO and plated Cu. An additional plating approach, using self-passivated aluminum as mask, allows to produce well-defined 30 mm wide Cu contacts on the PSC. Such a plating process allows for plating a low-resistive Cu grid simultaneously on both sides of a perovskite silicon heterojunction tandem solar cell with TCO, independent of substrate size.

Recently, hybrid processing using evaporation and spin-coating has been applied for the fabrication of perovskite silicon tandem solar cells with record power conversion efficiencies (PCEs) of 25.2%. To achieve large area, high-throughput production of solar cells, spray-coating, a well-known scalable method used in the industry, has advantages over spin-coating. Therefore, we apply a hybrid method using the evaporation of PbI2 and spraying of methylammonium iodide (MAI) for the fabrication of perovskite solar cells. This article presents a systematic study of sprayed MAI amount and processing parameters on the performance of solar cells. We find clear correlations between the processing parameters of the sprayed MAI, the crystallinity of CH3NH3PbI3 and the PCE of the resulting PSCs. High crystallinity and morphology of the CH3NH3PbI3 film is achieved using a slow nozzle speed of 30 mm·s−1. An average PCE of 11.6% ± 3.1% (maximum PCE of 14.3%, stabilized PCE of 10%) was achieved with a normalized MAI amount of 3.4, which represent the flow rate of 0.17 ml·min−1, nozzle speed of 30 mm·s−1, MAI concentration of 9 mg·mL−1, and one single spray pass. Moreover, we successfully show a proof-of-concept of this method for the deposition of homogenous perovskite layers on pyramidal textured silicon.

Monolithic perovskite silicon tandem solar cells can overcome the theoretical efficiency limit of silicon solar cells. This requires an optimum bandgap, high quantum efficiency, and high stability of the perovskite. Herein, a silicon heterojunction bottom cell is combined with a perovskite top cell, with an optimum bandgap of 1.68 amp; 8201;eV in planar p i n tandem configuration. A methylammonium free FA0.75Cs0.25Pb I0.8Br0.2 3 perovskite with high Cs content is investigated for improved stability. A 10 molarity increase to 1.1 amp; 8201;m of the perovskite precursor solution results in amp; 8776;75 amp; 8201;nm thicker absorber layers and 0.7 amp; 8201;mA amp; 8201;cm amp; 8722;2 higher short circuit current density. With the optimized absorber, tandem devices reach a high fill factor of 80 and up to 25.1 certified efficiency. The unencapsulated tandem device shows an efficiency improvement of 2.3 absolute over 5 amp; 8201;months, showing the robustness of the absorber against degradation. Moreover, a photoluminescence quantum yield analysis reveals that with adapted charge transport materials and surface passivation, along with improved antireflection measures, the high bandgap perovskite absorber has the potential for 30 tandem efficiency in the near future

In monolithic perovskite/silicon tandem solar cells, it is important to know which sub-cells is limiting the overall current to adapt the perovskite absorber thickness and bandgap accordingly. The current matching situation is usually analyzed by integrating measured external quantum efficiencies. However, this method can lead to significant errors and misinterpretations if meta-stable perovskite solar cells are involved. In this work, spectrometric characterization is presented as an alternative approach avoiding these errors. Current-voltage curves are recorded under different spectral conditions. Spectral irradiance settings are varied in a systematic way from red-shifted spectra (the perovskite top solar cell limits the current) to blue-shifted spectra (the silicon bottom solar cell limits the current) around the Air Mass 1.5 global (AM1.5g) spectrum. This method not only allows for accurate determination of the current matching point, but also gives quantitative insight in the behavior of the single sub-cells and their influence on the tandem performance. As different current mismatching also influences other global cell parameters, an example is presented where the current loss due to the current mismatch is partly compensated by a strong fill factor increase when the silicon solar cell limits the current, resulting in a high-power output also at the AM1.5g condition.