Abstract
The organic–inorganic lead halide hybrids comprising semiconducting perovskite components and organic modules have proven to be promising candidates for optoelectronic applications. The modulation of the inorganic components as optical centres by diverse organic cationic templates is under intense investigation. Herein, we successfully prepared new one-dimensional lead halide hybrid perovskites [L1]2n[Pb2Cl6]n∞·nH2O (1) and [PbBr2(L2)]n∞·0.5nH2O (2), and the dimeric complex [PbBr2(L3)]2 (3) in water media. In 1, 2-(2-hydroxyethyl)-2H-imidazo[1,5-a]pyridinium cation [L1]+ resulted from the oxidative condensation–cyclization between formaldehyde, ethanolamine and 2-pyridinecarbaldehyde (2-PCA); the polydentate Schiff base ligands L2 and L3 formed in the in situ condensation of 2-PCA and ethanolamine or ethylenediamine, respectively. The lead chloride hybrid 1 contains the previously unreported type of a [Pb2Cl6]∞ double chain constructed from three-edge- and five-edge-sharing PbCl6 octahedra, and cations forming π-bonded stacks aligned along the inorganic wires. In the crystal of 2, pairs of the double-side organically decorated [PbBr2(L2)]∞ chains built of corner-sharing PbBr3N2O octahedra arrange hydrophilic channels to host water molecules. In the solid state, the identically stacked dimers of 3 form columns parallel to the ab plane with the Pb2Br4 moieties in the column being strictly coplanar. Hirshfeld surface analysis was used to rationalize the packing patterns through hydrogen bonds of O−H···O/Cl and C−H···O/Cl types with the involvement of OH groups of [L1]+, L2 and water molecules in 1 and 2, as well as C–H∙∙∙Br hydrogen bonding in 2 and 3. The QTAIM analysis of non-covalent interactions in 1–3 was performed. According to the analysis of the solid-state UV–visible reflectance spectra by a Tauc plot, the optical band gap values of 1, 2 and 3 as direct gap semiconductors were estimated to be 3.36, 3.13 and 2.96 eV, respectively.
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