Highly crystalline MAPbI3 perovskite grain formation by irreversible poor-solvent diffusion aggregation, for efficient solar cell fabrication

• 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 MAPbI3 perovskite by exploiting diffusion aggregation processes. Isopropanol solution based methylammonium lead triiodide (MAPbI3) 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 PbI2 crystallites in the Pb rich shell with a single crystal MAPbI3 core in newly formed grains. After a week stirring, the same aggregated suspension exhibited grains with only single crystal MAPbI3 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 MAPbI3 solar cells were fabricated by dissolving the powder and applying it in a classical fabrication route. The MAPbI3 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.

Ämnesord

NATURVETENSKAP  -- Kemi -- Materialkemi (hsv//swe)

NATURAL SCIENCES  -- Chemical Sciences -- Materials Chemistry (hsv//eng)

TEKNIK OCH TEKNOLOGIER  -- Nanoteknik (hsv//swe)

ENGINEERING AND TECHNOLOGY  -- Nano-technology (hsv//eng)

Nyckelord

High-angle annular dark-field imaging

MAPbI3 crystal growth

Nano-beam electron diffraction

Perovskite solar cells

PL mapping

Crystal growth

Crystallites

Crystallization

Energy dispersive spectroscopy

Energy efficiency

Fabrication

Grain boundaries

Layered semiconductors

Lead compounds

Lead metallography

Morphology

Nanocrystalline materials

Optical properties

Perovskite

Shells (structures)

Single crystals

Solvents

Thin film solar cells

Thin films

Transmission electron microscopy

Vacuum evaporation

Crystalline thin films

Energy dispersive X ray spectroscopy

Flexible manufacturing

Grain boundary effects

Nanobeam electron diffraction

Scanning transmission electron microscopes

Solar cell fabrication

Solar cell performance

Crystal structure

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