Rapid Scalable Processing of Tin Oxide Transport Layers for Perovskite Solar Cells.

The development of scalable deposition methods for perovskite solar cell materials is critical to enable the commercialization of this nascent technology. Herein, we investigate the use and processing of nanoparticle SnO2 films as electron transport layers in perovskite solar cells and develop deposition methods for ultrasonic spray coating and slot-die coating, leading to photovoltaic device efficiencies over 19%. The effects of postprocessing treatments (thermal annealing, UV ozone, and O2 plasma) are then probed using structural and spectroscopic techniques to characterize the nature of the np-SnO2/perovskite interface. We show that a brief "hot air flow" method can be used to replace extended thermal annealing, confirming that this approach is compatible with high-throughput processing. Our results highlight the importance of interface management to minimize nonradiative losses and provide a deeper understanding of the processing requirements for large-area deposition of nanoparticle metal oxides.

High-Efficiency Spray-Coated Perovskite Solar Cells Utilizing Vacuum-Assisted Solution Processing.

We use ultrasonic spray-coating to fabricate cesium-containing triple-cation perovskite solar cells with a power-conversion efficiency of up to 17.8%. Our fabrication route involves a brief exposure of the partially wet spray-cast films to a low vacuum, a process that is used to control film crystallization. We show that films that are not vacuum-exposed are relatively rough and inhomogeneous, while vacuum-exposed films are smooth and consist of small and densely packed perovskite crystals. The process techniques developed here represent a step toward a scalable and industrially compatible manufacturing process capable of creating stable and high-performance perovskite solar cells.

Spray-cast multilayer perovskite solar cells with an active-area of 1.5 cm2.

We utilise spray-coating under ambient conditions to sequentially deposit compact-TiO2, mesoporous-TiO2, CH3NH3PbI(3-x)Clx perovskite and doped spiro-OMeTAD layers, creating a mesoporous standard architecture perovskite solar cell (PSC). The devices created had an average power conversion efficiency (PCE) of 9.2% and a peak PCE of 10.2%; values that compare favourably with control-devices fabricated by spin-casting that had an average efficiency of 11.4%. We show that our process can be used to create devices having an active-area of 1.5 cm2 having an independently verified efficiency of 6.6%. This work demonstrates the versatility of spray-coating as well as its potential as a method of manufacturing low-cost, large-area, efficient perovskite devices.

Nanoscale Mapping of Bromide Segregation on the Cross Sections of Complex Hybrid Perovskite Photovoltaic Films Using Secondary Electron Hyperspectral Imaging in a Scanning Electron Microscope.

Mixed halide (I/Br) complex organic/inorganic hybrid perovskite materials have attracted much attention recently because of their excellent photovoltaic properties. Although it has been proposed that their stability is linked to the chemical inhomogeneity of I/Br, no direct proof has been offered to date. Here, we report a new method, secondary electron hyperspectral imaging (SEHI), which allows direct imaging of the local variation in Br concentration in mixed halide (I/Br) organic/inorganic hybrid perovskites on a nanometric scale. We confirm the presence of a nonuniform Br distribution with variation in concentration within the grain interiors and boundaries and demonstrate how SEHI in conjunction with low-voltage scanning electron microscopy can enhance the understanding of the fundamental physics and materials science of organic/inorganic hybrid photovoltaics, illustrating its potential for research and development in "real-world" applications.