Multifunctional-material-integrated various properties have been an attractive research field. In spite of persistent explorations into such materials, the conditions of coexistence are still confused. Organic-inorganic hybrid compounds are appropratie for designing these materials because of both their rich properties and flexible compositions. Here, a perovskite-type organic-inorganic hybrid compound, (Hmpy)MnCl (1; Hmpy = N-methylpyrrolidinium), with temperature, light, and electric stimuli-response characteristics has been rationally designed and synthesized. This hybrid compound shows a dielectric anomaly, a broad dielectric dispersion of the temperature range from 296 to 400 K, and brilliant red fluorescence at 632 nm with a high quantum yield of 54.54% under UV excitation. The coexistence of temperature, optical, and electric multiple stimuli-response properties in 1 demonstrates that our finding has a profound influence on the further exploration of the novel multifunctional materials.

Molecular bistable switches (electrical switches "ON" and "OFF") represent a class of highly desirable intelligent materials due to their sensitive switchable responses, simple and environmentally friendly processing, light weight, and mechanical flexibility. In particular, these switches above room temperature with potential practical application are rarely reported. In this work, a new zigzag chained organic-inorganic hybrid compound [NH(CH)Br]CdBr (1), which displays rapidly sensitive dielectric switching reversibility and remarkable switching antifatigue, has been successfully synthesized. Systematic characterization including differential scanning calorimetry measurements (DSC), dielectric measurements, and variable-temperature structural analyses was performed to reveal the phase transition of 1. A couple of reversible heat anomaly peaks at 335.6/323.8 K with a large hysteresis (ca. 11.8 K) were observed in the DSC curve, indicating the first-order type of phase transition. 1 exhibits an obvious dielectric switching at around 327 K, which makes 1 a potential switchable dielectric material. Variable-temperature structural analyses show that the cationic order-disorder motion is the main attribution for the phase transition of 1.

Two hybrids (CHN)CdCl (1) and (CHN)CdCl (2) were synthesized by stoichiometric regulation of reactants. 1 with a one-dimensional chain-like structure shows a step-like dielectric anomaly at around 158 K. 2 with a layered structure undergoes a prominent phase transition in the vicinity of 182 K, accompanying obvious dielectric relaxation behavior in a broad temperature range. Systematic characterization, such as differential scanning calorimetry (DSC), single-crystal X-ray diffraction, and dielectric measurements, has demonstrated that the phase transitions of 1 and 2 are both attributable to the dynamic motion of the organic cation. Significantly, dimensionality modulation triggers the tunable dielectric responses in these two compounds. Thus, regulation of the phase transition temperature and dielectric responses in the various dimensions of the structure is a potentially effective method to construct tunable dielectric phase transition materials.

Three hybrids display tunable structural transitions, achieving the regulation of phase transition temperature and dielectric characteristics.