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Two new organic–inorganic hybrid molecular single crystals, 4-Iodoanilinium perchlorate 18-crown-6 (1) and 4-Iodoanilinium borofluorate 18-crown-6 (2), with large sizes and high thermal stability were successfully synthesized by solution method. Their structures, phase purities, thermal stability, dielectric, absorption and fluorescence spectra were systematically investigated for potential applications. Compounds 1 and 2 crystallize in orthorhombic crystal system, in same space group, namely Pnma. The thermal measurements shown 1 and 2 maintain high thermal stability up to 150 °C. The temperature dependency of dielectric constant was studied, and no distinct anomaly was observed. The band gap were calculated to be 3.38 eV and 3.57 eV for 1 and 2, respectively, slightly smaller than those of layer perovskite (benzylammonium)2PbCl4 semiconducting materials, which have potential applications in optoelectronic detection field. The investigations throw light on the semiconductor properties of organic–inorganic hybrid crown type material and provide two types of crown compounds with high thermal stability.

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Organic–inorganic hybrid new crystals, [(parachloroanilinum+)(18-crown-6)][ClO4−](CH3COCH3) and [(parachloroanilinum+)(18-crown-6)][BF4−](CH3COCH3), with high phase transition temperatures and noncentrosymmetric structures were grown. Their physical properties, including their structures, phase transitions, and dielectric, piezoelectric and photoluminescent properties, were systematically investigated. A phase transition at 71 °C was successively detected and confirmed by DSC and dielectric measurements. Piezoelectric features were clearly verified by piezoresponse force microscopy. Both compounds show strong and wide photoluminescent properties. All the results make the two compounds promising candidates for potential applications in the piezoelectric and optical fields.

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