Spin-reorientation-induced magnetodielectric coupling effects in two layered perovskite magnets

Huang, Bo; Zhang, Jianyu; Huang, Rui‐Kang; Chen, Ming-Kun; Xue, Wei; Zhang, Wei‐Xiong; Zeng, Ming‐Hua

doi:10.1039/c8sc02917b

Cited by 54 publications

(49 citation statements)

References 45 publications

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“…The ferromagnetic hysteresis loops for the two hybrid perovskites below the Curie temperature are shown in Figure c, d. For (PED)CuCl 4 , the magnetization nearly saturates at a value of 0.12 emu g −1 in a field of 2000 Oe at 2 K. However, (BED) 2 CuCl 6 on the other hand, has strong ferromagnetism. The magnetization nearly saturates at a value of 10 emu g −1 in a field of 2000 Oe at 2 K. The saturated magnetization of (BED) 2 CuCl 6 is comparable to the value reported in the literature …”

Section: Figuresupporting

confidence: 86%

“…The representative current–voltage traces of these crystals are provided in Figure a, b, which were used in determining the conductivity. These traces are linear at low bias, which suggests Ohmic contact between electrodes and the various crystals . Both crystals show a general trend that their conductivities increase with rising temperature.…”

Section: Figurementioning

confidence: 84%

“…Magnetic susceptibility was investigated in Cs 4 Mn 1− x Cu x Sb 2 Cl 12 ( x =0–1), which were dependent on the concentration of manganese and copper . Investigations on the spin‐reorientation and spin‐control in 2D hybrid perovskite may help to design new materials for future spintronics . Despite extensive investigations on perovskites, ferromagnets coupled with thermochromism has not been reported to date.…”

Section: Figurementioning

confidence: 99%

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Reversible Thermochromism and Strong Ferromagnetism in Two‐Dimensional Hybrid Perovskites

Sun

Liu

et al. 2019

Angew Chem Int Ed

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Two‐dimensional (2D) hybrid perovskites have shown many attractive properties associated with their soft lattices and multiple quantum well structure. Herein, we report the synthesis and characterization of two new multifunctional 2D hybrid perovskites, (PED)CuCl4 and (BED)2CuCl6, which show reversible thermochromic behavior, dramatic temperature‐dependent conductivity change, and strong ferromagnetism. Upon temperature change, the (PED)CuCl4 and (BED)2CuCl6 crystals exhibit a reversible color change between yellow and red‐brown. The associated structural changes were monitored by in situ temperature‐dependent powder X‐ray diffraction (PXRD). The (BED)2CuCl6 exhibits superior thermal stability, with a thermochromic working temperature up to 443 K. The conductivity of (BED)2CuCl6 changes over six orders of magnitude upon temperature change. The 2D perovskites exhibit ferromagnetic properties with Curie temperatures around 13 K.

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Section: Figuresupporting

confidence: 86%

Section: Figurementioning

confidence: 84%

Section: Figurementioning

confidence: 99%

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Reversible Thermochromism and Strong Ferromagnetism in Two‐Dimensional Hybrid Perovskites

Sun

Liu

et al. 2019

Angew Chem Int Ed

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“…In addition, crystals of the Cu 2+ salts ( C n CuCl4 ) show ferromagnetism below 8 K . Furthermore, C2CuCl4 has been reported to show anomalous dielectric properties, and has attracted a great deal of interest in the field of multiferroic materials . Owing to these unique properties, an enormous amount of research into the C n MX4 family has been published.…”

Section: Introductionmentioning

confidence: 99%

“…[25,26] Furthermore, C2CuCl4 has been reported to show anomalous dielectric properties, and has attracted a great deal of interesti nt he field of multiferroic materials. [27][28][29] Owing to these unique properties,a ne normousa mount of research into the CnMX4 family has been published. However, to the best of our knowledge,t he thermalc onductivities of CnMX4 salts in incommensurate phases have not been reported.…”

mentioning

confidence: 99%

Negative‐to‐Positive Thermal Conductivity Temperature Coefficient Transition Induced by Dynamic Fluctuations of the Alkyl Chains in the Layered Complex (C₄H₉NH₃)₂CuCl₄

Hoshino

Tamura

Akutagawa

2020

Chemistry A European J

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A negative‐to‐positive transition of the temperature coefficients of thermal conductivity was found in the two‐dimensional organic–inorganic layered complex (C4H9NH3)2CuCl4 (C4CuCl4) over the three structural phase transitions in the range 176–218 K. The coefficients of the low‐temperature phases (85–200 K, α and β phases) were negative, as is typical for insulating crystals, whereas those of the high‐temperature phases (200–300 K, γ and δ phases) were positive, as is typical for glasses and liquids. Single‐crystal X‐ray structure analyses revealed that the tilted C4H9NH3+ chains in the α and β phases were fully outstretched in the δ phase, and the interlayer distances between the CuCl42− planes increased significantly. The γ phase was an intermediate phase that crystallized with an incommensurate structure, in which the CuCl42− sheets formed wave‐like structures consisting of connected alternating regions of β‐like and δ‐like moieties. In the γ and δ phases, thermal fluctuations of the C4H9NH3+ chains were found in the electron density maps; however, powder X‐ray diffraction (PXRD) data indicated that the thermal expansion of the C4H9NH3+ layers was restricted by the rigid CuCl42− layers. This situation was considered to induce glass‐like thermal conducting properties in the material, such as a positive temperature coefficient. The mean free path of the phonons estimated by using the thermal conductivities and heat capacities was a function of T−1 in the range 85–200 K, as would be expected for crystals, whereas it was approximately constant in the range 200–300 K, which is typical of glasses. In addition, the existence of soft vibration modes in the two‐dimensional perovskite CuCl42− sheets was revealed by analysis of the incommensurate crystal structure of the γ phase. These low‐energy vibration modes were believed to induce the cooperative phase transitions, along with the thermal fluctuations and van der Waals interactions in the C4H9NH3+ layers.

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Magnetic Properties of Layered Hybrid Organic‐Inorganic Metal‐Halide Perovskites: Transition Metal, Organic Cation and Perovskite Phase Effects

Asensio

Marras

Spirito

et al. 2022

Adv Funct Materials

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Understanding the structural and magnetic properties in layered hybrid organic‐inorganic metal halide perovskites (HOIPs) is key for their design and integration in spin‐electronic devices. Here, a systematic study is conducted on ten compounds to understand the effect of the transition metal (Cu2+, Mn2+, Co2+), organic spacer (alkyl‐ and aryl‐ammonium), and perovskite phase (Ruddlesden‐Popper and Dion‐Jacobson) on the properties of these materials. Temperature‐dependent Raman measurements show that the crystals’ structural phase transitions are triggered by the motional freedom of the organic cations as well as by the flexibility of the inorganic metal‐halide lattice. In the case of Cu2+ HOIPs, an increase of the in‐plane anisotropy and a reduction of the octahedra interlayer distance is found to change the behavior of the HOIP from that of a 2D ferromagnet to that of a quasi‐3D antiferromagnet. Mn2+ HOIPs show inherent antiferromagnetic octahedra intralayer interactions and a phenomenologically rich magnetism, presenting spin‐canting, spin‐flop transitions, and metamagnetism controlled by the crystal anisotropy. Co2+ crystals with non‐linked tetrahedra show a dominant paramagnetic behavior irrespective of the organic spacer and the perovskite phase. This study demonstrates that the chemical flexibility of HOIPs can be exploited to develop novel layered magnetic materials with tailored magnetic properties.

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Spin-reorientation-induced magnetodielectric coupling effects in two layered perovskite magnets

Abstract: Spin-reorientation-induced magnetodielectric effects were discovered in two layered perovskite magnets, (C6H5CH2CH2NH3)2[MCl4] (M = Mn2+ and Cu2+), via highly reproducible isothermal magnetodielectric measurements on single-crystal samples.

Cited by 54 publications

References 45 publications

Reversible Thermochromism and Strong Ferromagnetism in Two‐Dimensional Hybrid Perovskites

Reversible Thermochromism and Strong Ferromagnetism in Two‐Dimensional Hybrid Perovskites

Negative‐to‐Positive Thermal Conductivity Temperature Coefficient Transition Induced by Dynamic Fluctuations of the Alkyl Chains in the Layered Complex (C₄H₉NH₃)₂CuCl₄

Magnetic Properties of Layered Hybrid Organic‐Inorganic Metal‐Halide Perovskites: Transition Metal, Organic Cation and Perovskite Phase Effects

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Spin-reorientation-induced magnetodielectric coupling effects in two layered perovskite magnets

Abstract: Spin-reorientation-induced magnetodielectric effects were discovered in two layered perovskite magnets, (C6H5CH2CH2NH3)2[MCl4] (M = Mn2+ and Cu2+), via highly reproducible isothermal magnetodielectric measurements on single-crystal samples.

Cited by 54 publications

References 45 publications

Reversible Thermochromism and Strong Ferromagnetism in Two‐Dimensional Hybrid Perovskites

Reversible Thermochromism and Strong Ferromagnetism in Two‐Dimensional Hybrid Perovskites

Negative‐to‐Positive Thermal Conductivity Temperature Coefficient Transition Induced by Dynamic Fluctuations of the Alkyl Chains in the Layered Complex (C4H9NH3)2CuCl4

Magnetic Properties of Layered Hybrid Organic‐Inorganic Metal‐Halide Perovskites: Transition Metal, Organic Cation and Perovskite Phase Effects

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Negative‐to‐Positive Thermal Conductivity Temperature Coefficient Transition Induced by Dynamic Fluctuations of the Alkyl Chains in the Layered Complex (C₄H₉NH₃)₂CuCl₄