Two Lead‐Free Organic‐Inorganic Hybrid Halides: Exploring Dielectric Switching and Photoluminescence Integrated in Crystals

Cao, Tengfei; Xiao, H.; Xu, Zihan; Ye, Liwang; Wang, Yuanjie; Zhuang, Xiuli

doi:10.1002/ejic.202100567

Cited by 9 publications

(3 citation statements)

References 65 publications

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“…Among these, the polyhedron with indium as central ions and halogen and water molecules as ligands [In X m (H 2 O) n , X = halogen anions, m + n = 6] are well known and have been extensively studied. The coordination number of indium can vary from four to seven by altering bond lengths of ligands. − This is in particular true when indium is coordinated with halogen anions and oxygen in water molecules, among which the latter bond is relatively weak. This allows the whole framework to not collapse if the water molecules are ionized (loss of protons) or even removed.…”

Section: Introductionmentioning

confidence: 99%

High, Multiple, and Nonvolatile Polarizations in Organic–Inorganic Hybrid [(CH₃)₃(CH₂CH₂Cl)N]₂InCl₅·H₂O for Memcapacitor

Lu,

Luo,

Zhou

et al. 2023

J. Am. Chem. Soc.

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Dielectrics with high, nonvolatile, and multiple polarizations are required for fabricating memcapacitors that enable high parallelism and low energy consumption in artificial neuromorphic computing systems as artificial synapses. Conventional ferroelectric materials based on displacive and order−disorder types generally have difficulty meeting these requirements due to their low polarization values (∼150 μC/cm 2 ) and persistent electrical hysteresis loops. In this study, we report a novel organic−inorganic hybrid (CETM) 2 InCl 5 •H 2 O (CETM = (CH 3 ) 3 (CH 2 CH 2 Cl)N) exhibiting an intriguing polarization vs electric field (charge vs voltage) "hysteresis loop" and a record-high nonvolatile polarization over 30 000 μC/cm 2 at room temperature. The polarization is highly dependent on the period and amplitude of the ac voltage, showing multiple nonvolatile states. Electrochemical impedance spectroscopy, time-dependent current behavior, disparate resistor response in the dehydrated derivative (CETM) 2 InCl 5 , and the negative temperature dependence of ionic conductance support that the memcapacitor behavior of (CETM) 2 InCl 5 •H 2 O stems from irreversible longrange migration of protons. First-principles calculations further confirm this and clarify the microscale mechanism of anisotropic polarization response. Our findings may open up a new avenue for developing memcapacitors by harnessing the benefits of ion migration in organic−inorganic hybrids.

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Section: Introductionmentioning

confidence: 99%

High, Multiple, and Nonvolatile Polarizations in Organic–Inorganic Hybrid [(CH₃)₃(CH₂CH₂Cl)N]₂InCl₅·H₂O for Memcapacitor

Lu,

Luo,

Zhou

et al. 2023

J. Am. Chem. Soc.

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“…Furthermore, it is found that the In(III) atom and different kinds of halogens can form diverse indium halide anions, which can combine with organic ammonium to generate inorganic–organic hybrid compounds A n –3 [In III X n ] (A = organic ammonium cation) with various structures and different compositions. − Jakubas et al. obtained two alkylammonium halogenoindium(III) phase transition materials, [(C 2 H 5 ) 4 N]InBr 4 and [(CH 3 ) 4 N]InBr 4 , with T p values of 225 and 186 K, respectively.…”

Section: Introductionmentioning

confidence: 99%

Two In-based Hybrid Compounds with Structural Phase Transitions Caused by Displacement Motion or Dynamic Disorder

Wang,

Luo,

2023

Crystal Growth & Design

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Inorganic−organic hybrid phase transition compounds have been widely studied because of their abundant physical properties and excellent chemical tunability. In this work, two novel inorganic−organic hybrid In(III)-based phase transition compounds, (C 10 H 16 N) 2 [InBr 5 (H 2 O)] (1, C 10 H 16 N + = 4-phenylbutylammonium) and (C 6 H 14 N)[InBr 4 ] (2, C 6 H 14 N + = Nmethylpiperidinium), have been obtained and studied. Differential scanning calorimetry (DSC) tests show that 1 and 2 experience phase transitions with a T p (phase transition temperature) of 260 and 304 K, respectively. Single-crystal diffraction analysis reveals that the source of the phase transition of 1 is the displacement of (C 10 H 16 N) + cations. The reversible phase transition of 2 is triggered by the change of the disorder degree in the (C 6 H 14 N) + cations. Meanwhile, compounds 1 and 2 display distinct dielectric response behavior near T p . This study will provide valuable insights for further investigation and exploration of the novel In(III)based inorganic−organic hybrid phase transition composites.

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“…[23][24][25][26][27][28][29][30][31][32][33] Recently, zinc halides hybrids with stable oxidation states have attracted some attention due to their unique photophysical properties. [34][35][36][37] It is worth noting that replacing toxic Pb 2+ with "green" Zn 2+ significantly reduces the harm to the environment and humans. [38][39][40] For example, based on the compositional engineering strategy, Zhou and co-workers prepared several zinc metal halide: A 2 ZnX 4 (A = Rb, Cs; X = Cl, Br) with or without Cu-doping and their mixed-halide counterparts (Cs 2 ZnCl x Br 4-x :Cu, x = 0−4), blue emitting Cs 2 ZnBr 4 :Cu with a high photoluminescent quantum yield (PLQY) of 57%.…”

Section: Introductionmentioning

confidence: 99%

Zero‐Dimensional Organic–Inorganic Hybrid Zinc Halides for Multiple Applications in Anti‐Counterfeiting, X‐Ray Imaging and White LEDs

Wang,

Zhou,

Chen

et al. 2023

Advanced Optical Materials

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Zinc halides have been less explored even though they are a promising lead‐free family with the merits of environmental friendliness and low cost. Here, the organic–inorganic hybrid zinc halides are screened with aromatic molecules containing amino groups (MXDA: m‐Xylylenediamine, ABI: 2‐Aminobenzimidazole, pipda: 2‐piperidylmethylamine, p‐MPEA: p‐Methylphenethylamine), and six new compounds are discovered: (MXDA)ZnCl4 (1), (ABI)2ZnCl4 (2), (pipda)2H2OZnCl2 (3), [(pipda)4Zn2Br4]·H2O (4), (p‐MPEA)2ZnCl4 (5), and (p‐MPEA)2ZnBr4 (6). The discovered compounds exhibit diverse efficient light emissions (blue, green, yellow, and ultraviolet) under ultraviolet light irradiation. By doping Sb and Mn at the Zn site, (MXDA)ZnCl4 exhibits different colors of light under excitation light of different wavelengths, so it is successfully used for anti‐counterfeiting. (MXDA)Zn0.91Mn0.09Cl4 is also found to be an efficient X‐ray scintillator for X‐ray imaging. Among the as‐explored new phases, a maximum photoluminescent quantum yield of 82.60% is realized, enabling the utilization for white light‐emitting diodes. The results suggest that the zinc halides are a new lead‐free family with superior optoelectronic properties, which can be used for multiple applications.

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Two Lead‐Free Organic‐Inorganic Hybrid Halides: Exploring Dielectric Switching and Photoluminescence Integrated in Crystals

Cited by 9 publications

References 65 publications

High, Multiple, and Nonvolatile Polarizations in Organic–Inorganic Hybrid [(CH₃)₃(CH₂CH₂Cl)N]₂InCl₅·H₂O for Memcapacitor

High, Multiple, and Nonvolatile Polarizations in Organic–Inorganic Hybrid [(CH₃)₃(CH₂CH₂Cl)N]₂InCl₅·H₂O for Memcapacitor

Two In-based Hybrid Compounds with Structural Phase Transitions Caused by Displacement Motion or Dynamic Disorder

Zero‐Dimensional Organic–Inorganic Hybrid Zinc Halides for Multiple Applications in Anti‐Counterfeiting, X‐Ray Imaging and White LEDs

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Two Lead‐Free Organic‐Inorganic Hybrid Halides: Exploring Dielectric Switching and Photoluminescence Integrated in Crystals

Cited by 9 publications

References 65 publications

High, Multiple, and Nonvolatile Polarizations in Organic–Inorganic Hybrid [(CH3)3(CH2CH2Cl)N]2InCl5·H2O for Memcapacitor

High, Multiple, and Nonvolatile Polarizations in Organic–Inorganic Hybrid [(CH3)3(CH2CH2Cl)N]2InCl5·H2O for Memcapacitor

Two In-based Hybrid Compounds with Structural Phase Transitions Caused by Displacement Motion or Dynamic Disorder

Zero‐Dimensional Organic–Inorganic Hybrid Zinc Halides for Multiple Applications in Anti‐Counterfeiting, X‐Ray Imaging and White LEDs

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Product

Resources

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High, Multiple, and Nonvolatile Polarizations in Organic–Inorganic Hybrid [(CH₃)₃(CH₂CH₂Cl)N]₂InCl₅·H₂O for Memcapacitor

High, Multiple, and Nonvolatile Polarizations in Organic–Inorganic Hybrid [(CH₃)₃(CH₂CH₂Cl)N]₂InCl₅·H₂O for Memcapacitor