Yamamoto, T; Oswald, IWH; Savory, CN; Ohmi, T; Koegel, AA; Scanlon, DO; Kageyama, H; Yamamoto, T; Oswald, IWH; Savory, CN; Ohmi, T; Koegel, AA; Scanlon, DO; Kageyama, H; Neilson, JR; - view fewer (2020) Structure and Optical Properties of Layered Perovskite (MA)₂PbI₂–ₓBrₓ(SCN)₂ (0 ≤ x < 1.6). Inorganic Chemistry , 59 (23) pp. 17379-17384. 10.1021/acs.inorgchem.0c02686.

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Abstract

The layered perovskite (MA)_{2}PbI_{2}(SCN)_{2} (MA = CH_{3}NH_{3}^{+}) is a member of an emerging series of compounds derived from hybrid organic-inorganic perovskites. Here, we successfully synthesized (MA)_{2}PbI_{2}-_{x}Br_{x}(SCN)_{2} (0 ≤ x < 1.6) by using a solid-state reaction. Despite smaller bromide substitution for iodine, 1% linear expansion along the a axis was observed at x ∼ 0.4 due to a change of the orientation of the SCN- anions. Diffuse reflectance spectra reveal that the optical band gap increases by the bromide substitution, which is supported by the DFT calculations. Curiously, bromine-rich compounds where x ≥ 0.8 are light sensitive, leading to partial decomposition after ∼24 h. This study demonstrates that the layered perovskite (MA)_{2}PbI_{2}(SCN)_{2} tolerates a wide range of bromide substitution toward tuning the band gap energy.

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