Abstract
Energy efficient synthesis providing high quality crystalline thin films are highly desired in many applications. Here we devise a non-toxic solvent approach for production of highly crystalline MAPbI 3 perovskite by exploiting diffusion aggregation processes. Isopropanol solution based methylammonium lead triiodide (MAPbI 3 ) is used in this context, where the crystal growth initiation starts in an unstable suspension far from equilibrium and the subsequent crystallization is driven by the solubility parameters. The crystal formation is monitored by scanning transmission electron microscope (STEM), observing small crystallization centers growing as time evolves to large grains with high crystal purity. Energy dispersive X-ray spectroscopy (EDS) in STEM mode revealed a Pb rich core-shell structure in newly formed grains. Nano-beam Electron Diffraction (NBED) scan defined PbI 2 crystallites in the Pb rich shell with a single crystal MAPbI 3 core in newly formed grains. After a week stirring, the same aggregated suspension exhibited grains with only single crystal MAPbI 3 structure. The NBED analysis shows a kinetically slow transition from a core shell structure to a single crystal grain. This research presents an impactful insight on the factors that may cause sub-stoichiometric grain boundary effects which can influence the solar cell performance. In addition, the structure, morphology and optical properties of the perovskite grains have been presented. A powder of highly crystalline particles was subsequently prepared by evaporation of the solvent in a low-vacuum oven. Thin film MAPbI 3 solar cells were fabricated by dissolving the powder and applying it in a classical fabrication route. The MAPbI 3 solar cells gave a champion efficiency of 20% (19.9%) and an average efficiency at approximately 17% with low hysteresis effects. Here a strategy to manufacture the material structure without toxic solvents is highlighted. The single-crystal growth devised here opens both for shelf storage of materials as well as a more flexible manufacturing of devices. The process can likely be extended to other fields, where the intermediate porous framework and large surface area would be beneficial for battery or super capacitor materials. • A non-toxic solvent approach for production of high quality MAPbI 3 perovskite grains. • Nano-beam electron diffraction scan on PbI 2 crystallites and single crystal MAPbI 3 grains. • The porous framework of grains and large surface area would be beneficial for energy storage. • Low hysteresis effects and high efficiency for the perovskite solar cells.
Highlights
Finding new routes for low energy synthesis of materials promising for energy conversion and storage is a necessary and a rigorous task
From the Nano-beam Electron Diffraction (NBED) analysis, the results proposed an interfacial nanostructure which con sists of the salt PbI2 with band gap 2.3 eV and MA+ and I− ions, each quantum well in the semiconducting salts set up new selection rule that affect the conditions for charges to flow through the structure
We have explored an approach for production of high quality MAPbI3 perovskite powder using only non-toxic solvent, isopropanol
Summary
Finding new routes for low energy synthesis of materials promising for energy conversion and storage is a necessary and a rigorous task. The lead halide (APbX3) perovskites have reached impressively high efficiency in solar cells in the last years [1,2,3] These materials are promising candidates in light emitting diodes [4,5,6], lasing applications [7,8] and solar-to-fuel energy conversion devices [9,10], due to their unique optical and electronic properties. One advantage with the perovskite material is the ability to obtain high crystallinity at comparably low temperatures With advanced techniques such as grazing-incidence small-angle scattering and wideangle scattering the crystallization behavior, crystal orientation and structural phase transitions in new synthesis routes can be observed and tuned with additives [11]. Solidification and crystallization of a solution determines the final properties to a large extent, and by studying the formation mechanism it can be controlled in future structure designs [13]
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