Physically and Chemically Stable Molybdenum-Based Composite Electrodes for p-i-n Perovskite Solar Cells.

Metal halide perovskite solar cells (PSCs) have garnered much attention in recent years. Despite the remarkable advancements in PSCs utilizing traditional metal electrodes, challenges such as stability concerns and elevated costs have necessitated the exploration of innovative electrode designs to facilitate industrial commercialization. Herein, a physically and chemically stable molybdenum (Mo) electrode is developed to fundamentally tackle the instability factors introduced by electrodes. The combined spatially resolved element analyses and theoretical study demonstrate the high diffusion barrier of Mo ions within the device. Structural and morphology characterization also reveals the negligible plastic deformation and halide-metal reaction during aging when Mo is in contact with perovskite (PVSK). The electrode/underlayer junction is further stabilized by a thin seed layer of titanium (Ti) to improve Mo film's uniformity and adhesion. Based on a corresponding p-i-n PSCs (ITO/PTAA/PVSK/C60/SnO2/ITO/Ti/Mo), the champion sample could deliver an efficiency of 22.25%, which is among the highest value for PSCs based on Mo electrodes. Meanwhile, the device shows negligible performance decay after 2000 h operation, and retains 91% of the initial value after 1300 h at 50-60 °C. In summary, the multilayer Mo electrode opens an effective avenue to all-round stable electrode design in high-performance PSCs.

Isolating the Oxygen Adsorption Defects on Sputtered Tin Oxide for Efficient Perovskite Solar Cells.

Tin oxide (SnO2) is the most commonly used electron transport material for perovskite solar cells (PSCs). Various techniques have been applied to deposit tin dioxide, including spin-coating, chemical bath deposition, and magnetron sputtering. Among them, magnetron sputtering is one of the most mature industrial deposition techniques. However, PSCs based on magnetron-sputtered tin oxide (sp-SnO2) have a lower open-circuit voltage (Voc) and power conversion efficiency (PCE) than those prepared by the mainstream solution method. This is mainly due to the oxygen-related defects at the sp-SnO2/perovskite interface, and traditional passivation strategies usually have little effect on them. Herein, we successfully isolate the oxygen adsorption (Oads) defects located on the surface of sp-SnO2 from the perovskite layer using a PCBM double-electron transport layer. This isolation strategy effectively suppresses the Shockley-Read-Hall recombination at the sp-SnO2/perovskite interface, which results in an increase in the Voc from 0.93 to 1.15 V and an increase in PCE from 16.66 to 21.65%. To our knowledge, this is the highest PCE achieved using a magnetron-sputtered charge transport layer to date. The unencapsulated devices maintain 92% of their initial PCE after storage in air with a relative humidity of 30-50% after 750 h. We further use the solar cell capacitance simulator (1D-SCAPS) to confirm the effectiveness of the isolation strategy. This work highlights the application prospect of magnetron sputtering in the field of perovskite solar cells and provides a simple yet effective way to tackle the interfacial defect issue.

Doping Mechanism of Perovskite Films with PbCl2 Prepared by Magnetron Sputtering for Enhanced Efficiency of Solar Cells.

The last decade has witnessed a rapid growth of perovskite solar cells extended from mesoporous to planar architecture as well as from solution processing to solvent-free fabrication. The preparation of perovskite films by solvent-free method still presents significant challenges, such as the difficulty of film preparation by multiple evaporation sources in vapor deposition and the immaturity of the sputtered method. Here, we present a planar perovskite solar cell fabricated by solvent-free magnetron sputtering without the assistance of the mesoporous TiO2 layer, and lead chloride (PbCl2) was mechanically milled into the target of methylammonium lead halides (MAPbI3) to improve the quality of perovskite film by regulating the crystallization process with the Cl element. Furthermore, the internal reason for the effect of different PbCl2 doping contents on the trap density of perovskite films was also investigated in detail. These lead to an improved power conversion efficiency of planar heterojunction perovskite solar cells up to 17.10%, which is the highest efficiency recorded for the sputtered perovskite solar cells so far. The stability of resulting solar cells has also been significantly improved by exploring the doping mechanism of perovskite films with PbCl2 in detail, showing great research and application prospect.

Organic-Inorganic Perovskite Films and Efficient Planar Heterojunction Solar Cells by Magnetron Sputtering.

Organic-inorganic halide perovskites have been widely used in photovoltaic technologies. Despite tremendous progress in their efficiency and stability, perovskite solar cells (PSCs) are still facing the challenges of upscaling and stability for practical applications. As a mature film preparation technology, magnetron sputtering has been widely used to prepare metals, metallic oxides, and some semiconductor films, which has great application potential in the fabrication of PSCs. Here, a unique technology where high-quality perovskite films are prepared via magnetron sputtering for controllable composition, solvent-free, large-area, and massive production, is presented. This strategy transforms the perovskite materials from powder to thin films by magnetron sputtering and post-treatment (vapor-assisted treatment with methanaminium iodide gas and methylamine gas treatment), which is greatly favorable to manufacture tandem solar cells. The power conversion efficiency (PCE) of PSCs with perovskite films fabricated by magnetron sputtering is 6.14%. After optimization, high-performance perovskite films with excellent electronic properties are obtained and stable PSCs with excellent reproducibility are realized, showing a PCE of up to 15.22%. The entirely novel synthetic approach opens up a new and promising way to achieve high-throughput magnetron sputtering for large-area production in commercial applications of planar heterojunction and tandem PSCs.

Mechanochemical synthesis of pure phase mixed-cation/anion (FAPbI3) x (MAPbBr3)1-x hybrid perovskite materials: compositional engineering and photovoltaic performance.

Organic-inorganic hybrid perovskites have emerged as promising light harvesting materials for many optoelectronic devices. Here, we present a facile mechanochemical synthesis (MCS) route for the preparation of a series of pure phase mixed-cation/anion (FAPbI3) x (MAPbBr3)1-x (0 ≤ x ≤ 1) hybrid perovskite materials for high-efficiency thin-film perovskite solar cells (PSCs). The use of (α-FAPbI3)0.95(MAPbBr3)0.05 perovskite prepared by MCS for the thin-film PSCs achieves a maximum PCE of 15.9% from a current-voltage (J-V) scan, which stabilises at 15.4% after 120 s of the maximum power point output. Furthermore, PSCs based on (KPbI3)0.05(FAPbI3)0.9(MAPbBr3)0.05 perovskite prepared by MCS exhibit higher photovoltaic performance and lower hysteresis compared with (α-FAPbI3)0.95(MAPbBr3)0.05, with a maximum PCE of 16.7%. These results indicate that the use of mechanochemically synthesised perovskites provides a promising strategy for high performance PSCs and superior control in optoelectronic properties, leading to improved control in fabrication approaches and facilitating the development of efficient and stable PSCs in the future.

Solvent-Free Mechanochemical Synthesis of a Systematic Series of Pure-Phase Mixed-Halide Perovskites MAPb(Ix Br1-x )3 and MAPb(Brx Cl1-x )3 for Continuous Composition and Band-Gap Tuning.

Hybrid perovskites have recently received much attention in optoelectronic applications. However, hybrid perovskites are unstable in a humid environment. Mixed halide perovskites (MHPs) show enhanced stability and band-gap tunability upon engineering of their halide composition. Here, MHPs are prepared through a solvent-free mechanochemical synthesis (MCS) route that allows superior control over halide compositions than the solvent synthesis routes (SS). The MCS route eliminates the problem in the preparation of MAPb(Ix Br1-x )3 with continuously varying x, while maintaining the material properties and suppressing phase segregation present in SS routes. UV-vis absorption and X-ray diffraction patterns confirm the production of the desired pure-phase MHPs. For MAPb(Ix Br1-x )3 (0≤x≤1), with increased ratio of halide (x), the cubic phase gradually transforms into the tetragonal phase and band-gap tunability is accomplished. The MCS route for the preparation of MHPs is a very promising and efficient technique for superior control in optoelectronic properties, leading to improved control in fabrication approaches.