Controlled growth of perovskite layers with volatile alkylammonium chlorides

Jaewang Park, Jongbeom Kim, Hyun-Sung Yun, Min Jae Paik, Eunseo Noh, Hyun Jung Mun, Min Gyu Kim (), Tae Joo Shin () and Sang Il Seok ()
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Jaewang Park: Ulsan National Institute of Science and Technology (UNIST)
Jongbeom Kim: Ulsan National Institute of Science and Technology (UNIST)
Hyun-Sung Yun: Ulsan National Institute of Science and Technology (UNIST)
Min Jae Paik: Ulsan National Institute of Science and Technology (UNIST)
Eunseo Noh: Ulsan National Institute of Science and Technology (UNIST)
Hyun Jung Mun: Chonnam National University
Min Gyu Kim: Pohang University of Science and Technology (POSTECH)
Tae Joo Shin: Ulsan National Institute of Science and Technology (UNIST)
Sang Il Seok: Ulsan National Institute of Science and Technology (UNIST)

Nature, 2023, vol. 616, issue 7958, 724-730

Abstract: Abstract Controlling the crystallinity and surface morphology of perovskite layers by methods such as solvent engineering1,2 and methylammonium chloride addition3–7 is an effective strategy for achieving high-efficiency perovskite solar cells. In particular, it is essential to deposit α-formamidinium lead iodide (FAPbI3) perovskite thin films with few defects due to their excellent crystallinity and large grain size. Here we report the controlled crystallization of perovskite thin films with the combination of alkylammonium chlorides (RACl) added to FAPbI3. The δ-phase to α-phase transition of FAPbI3 and the crystallization process and surface morphology of the perovskite thin films coated with RACl under various conditions were investigated through in situ grazing-incidence wide-angle X-ray diffraction and scanning electron microscopy. RACl added to the precursor solution was believed to be easily volatilized during coating and annealing owing to dissociation into RA0 and HCl with deprotonation of RA+ induced by RA⋯H+-Cl− binding to PbI2 in FAPbI3. Thus, the type and amount of RACl determined the δ-phase to α-phase transition rate, crystallinity, preferred orientation and surface morphology of the final α-FAPbI3. The resulting perovskite thin layers facilitated the fabrication of perovskite solar cells with a power-conversion efficiency of 26.08% (certified 25.73%) under standard illumination.

Date: 2023
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DOI: 10.1038/s41586-023-05825-y

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