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Tailoring the coercive field in ferroelectric metal-free perovskites by hydrogen bonding.

ABSTRACT: The miniaturization of ferroelectric devices in non-volatile memories requires the device to maintain stable switching behavior as the thickness scales down to nanometer scale, which requires the coercive field to be sufficiently large. Recently discovered metal-free perovskites exhibit advantages such as structural tunability and solution-processability, but they are disadvantaged by a lower coercive field compared to inorganic perovskites. Herein, we demonstrate that the coercive field (110 kV/cm) in metal-free ferroelectric perovskite MDABCO-NH₄-(PF₆)₃ (MDABCO = N-methyl-N'-diazabicyclo[2.2.2]octonium) is one order larger than MDABCO-NH₄-I₃ (12 kV/cm) owing to the stronger intermolecular hydrogen bonding in the former. Using isotope experiments, the ferroelectric-to-paraelectric phase transition temperature and coercive field are verified to be strongly influenced by hydrogen bonds. Our work highlights that the coercive field of organic ferroelectrics can be tailored by tuning the strength of hydrogen bonding.

SUBMITTER: Choi HS

PROVIDER: S-EPMC8831526 | biostudies-literature | 2022 Feb

REPOSITORIES: biostudies-literature

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Tailoring the coercive field in ferroelectric metal-free perovskites by hydrogen bonding.

Choi Hwa Seob HS Li Shunning S Park In-Hyeok IH Liew Weng Heng WH Zhu Ziyu Z Kwon Ki Chang KC Wang Lin L Oh In-Hwan IH Zheng Shisheng S Su Chenliang C Xu Qing-Hua QH Yao Kui K Pan Feng F Loh Kian Ping KP

Nature communications 20220210 1

The miniaturization of ferroelectric devices in non-volatile memories requires the device to maintain stable switching behavior as the thickness scales down to nanometer scale, which requires the coercive field to be sufficiently large. Recently discovered metal-free perovskites exhibit advantages such as structural tunability and solution-processability, but they are disadvantaged by a lower coercive field compared to inorganic perovskites. Herein, we demonstrate that the coercive field (110 kV ...[more]

PMID: 35145089

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Project description:The oxohydroxoferrates(III) A 2[Fe2O3(OH)2] (A=K, Rb, Cs) were synthesized under hydroflux conditions. Approximately equimolar mixtures of the alkali metal hydroxides and water were reacted with Fe(NO3)3 ⋅ 9H2O at about 200 °C. The product formation depends on the hydroxide concentration, therefore also other reaction products, such as KFeO2, K2-x[Fe4O7-x(OH)x] or α-Fe2O3, are obtained. The crystal structures of the oxohydroxoferrates(III) A 2[Fe2O3(OH)2] follow the same structural principle, yet differ in their layer stacking or/and their hydrogen bonding systems depending on A and temperature. In the resulting four different orthorhombic structure types, [FeO3OH]4- tetrahedra share their oxide corners to create folded ∞ 2 [ Fe2O3(OH)2]2- layers. The terminal hydroxide ligands form hydrogen bonds between and/or within the layers. The positions of the hydrogen atoms in these networks are correlated. The A + cations are located between the folded anionic layers as well as in their trenches. Under reaction conditions, the potassium compound crystallizes in the space group Cmce (Pearson symbol oC88), showing a bimodal disorder of the hydrogen atoms in hydrogen bridges. In a virtually hysteresis-less first-order transition at 340(2) K, the structure slightly distorts into the room-temperature modification with the subgroup Pbca (oP88), and the hydrogen atoms order. The rubidium and caesium compounds are isostructural to each other but not to the potassium compound, and are always obtained as mixtures of two modifications with space groups Cmce (oC88') and Immb (oI88). Upon heating, the oxohydroxoferrates decompose into their anhydrides AFeO2 and water. The type of hydrogen bonding network influences the decomposition temperature, the structure and the morphology of the crystals. Despite the presence of iron(III), which was confirmed by 57Fe-Mössbauer spectroscopy, K2[Fe2O3(OH)2] is diamagnetic in the investigated temperature range between 1.8 and 300 K. Neutron diffraction revealed strong antiferromagnetic coupling of the magnetic moments, which are inverted in neighboring tetrahedra.

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Tailoring the coercive field in ferroelectric metal-free perovskites by hydrogen bonding.

Publications

Tailoring the coercive field in ferroelectric metal-free perovskites by hydrogen bonding.

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