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Synthesis and Characterization of (FA)3(HEA)2Pb3I11: A Rare Example of <1 1 0>-Oriented Multilayered Halide Perovskites

Abstract : Metal-halide perovskites have recently demonstrated great potential for a wide variety of optoelectronic applications, with their layered subfamily offering improved stability as compared to their 3D analogs. Among the layered compounds, subclass of <1 0 0> terminated compounds are currently dominating the field, while <1 1 0> subclass is comparably much less explored. Here we report on the synthesis of (FA) 3 (HEA) 2 Pb 3 I 11 obtained by room-temperature liquid-gas diffusion involving the intermediate-size cation hydroxyethylammonium (HEA +), formamidinium (FA +) and PbI 2 dissolved in an acidic solution. This multilayered hybrid perovskite is a rare example of a m= 3 member of the <1 1 0>-oriented series (A') 2 (A) m B m X 3m+2. Structural characterization based on X-ray diffraction and NMR investigations reveals that the small size cation FA + is located both in the inner layer of the perovskite sheet, but also in the interlayer space, while the intermediate-size cation HEA + is situated in the outer cavities of the perovskite sheet. (FA) 3 (HEA) 2 Pb 3 I 11 exhibits a broad absorption band in the visible region (400-650 nm) leading to an optical band gap of 1.96 eV. Electronic structure calculations confirm the direct nature of the band gap and evidence sizeable inter layer electronic coupling related to short I…I distances. These features are reminiscent of those observed for <1 0 0>-oriented Pb 3 I 10 analogs that have shown photovoltaic efficiencies over 18%. These findings should prompt further investigations for the design of other <1 1 0>-oriented multilayered (m= 3, 4,…) metal halide perovskites.
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https://hal.archives-ouvertes.fr/hal-03709286
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Soumis le : mercredi 29 juin 2022 - 18:09:21
Dernière modification le : mercredi 13 juillet 2022 - 13:19:20

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Maroua Ben Haj Salah, Nicolas Mercier, Magali Allain, Antonin Leblanc, Jens Dittmer, et al.. Synthesis and Characterization of (FA)3(HEA)2Pb3I11: A Rare Example of <1 1 0>-Oriented Multilayered Halide Perovskites. Chemistry of Materials, American Chemical Society, In press, ⟨10.1021/acs.chemmater.2c00130⟩. ⟨hal-03709286⟩

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