Magnetic field-temperature phase diagram of multiferroic (NH4)2FeCl5·H2O

Clune, Amanda; Nam, Jae Do; Lee, Minseong; Hughey, Kendall D.; Fernandez-Baca, J. A.; Fishman, Randy Scott; Singleton, John; Lee, Jun Hee; Musfeldt, J. L.

doi:10.1038/s41535-019-0180-1

Cited by 16 publications

(33 citation statements)

References 66 publications

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“…9. Pure (NH 4 ) 2 [FeCl 5 (H 2 O)] is a type-II multiferroic, which has been characterized in detail 13,25,27,29 . For x = 0.06 we still find a two-step magnetic ordering transition (T N = 7.25 K, T C = 7 K), which is typical for multiferroics with a cycloidal spin texture.…”

Section: B Low-temperature Transitionsmentioning

confidence: 99%

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Magnetoelectric coupling in the mixed erythrosiderite [(NH4)1−xKx]<

et al. 2020

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We present a study of the dielectric, structural, and magnetic properties of the multiferroic or linear magnetoelectric substitution series [(NH4)1−xKx]2[FeCl5(H2O)]. Pyroelectric currents, magnetic susceptibilities, and thermodynamic properties were examined on large single crystals of the erythrosiderite compounds and detailed magnetic-field versus temperature phase diagrams are derived for three different substitution levels. With increasing potassium concentration the material is tuned from a multiferroic (x ≤ 0.06) to a linear magnetoelectric (x ≥ 0.15) ground state. In contrast to the respective pure parent compounds with x = 0 or 1, however, the ferroelectric or linear magnetoelectric polarization in none of the substituted samples is switchable by external electric fields, because these samples exhibit a significant electric polarization already above the magnetic ordering transition. The polarization arises at a higher-lying structural phase transition that is examined by THz spectroscopy and, on a deuterated pure single crystal, by comprehensive neutron-diffraction experiments. The structural phase transition is attributed to an ordering of NH + 4 tetrahedra but does not break inversion symmetry in the pure material, while a finite K content causes pyroelectricity.

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Section: B Low-temperature Transitionsmentioning

confidence: 99%

“…This transition shows strong magnetoelastic coupling 13,28 and in the high-field regime the polarization can be explained with the p-d hybridization mechanism 27 . Magnetic saturation is reached around 30 T 29 . K 2 [FeCl 5 (H 2 O)] exhibits collinear antiferromagnetic order below T N = 14.3 K 14,30 .…”

Section: Introductionmentioning

confidence: 99%

Magnetoelectric coupling in the mixed erythrosiderite [(NH4)1−xKx]<

et al. 2020

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“…10. Pure (NH 4 ) 2 [FeCl 5 (H 2 O)] is a type-II multiferroic, which has been characterized in detail [15,27,29,31]. For x = 0.06 we still find a two-step magnetic ordering transition (T N = 7.25 K, T C = 7 K), which is typical for multiferroics with a cycloidal spin texture.…”

Section: B Low-temperature Transitionsmentioning

confidence: 85%

“…This transition shows strong magnetoelastic coupling [15,30] and in the high-field regime the polarization can be explained with the p-d hybridization mechanism [29]. Magnetic saturation is reached around 30T [31]. K 2 [FeCl 5 (H 2 O)] exhibits collinear antiferromagnetic order below T N = 14.3K [16,32].…”

Section: Introductionmentioning

confidence: 99%

Domain switching and exchange bias control by electric field in the multiferroic conical magnet Mn2GeO4

2020

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We present a study of the dielectric, structural, and magnetic properties of the multiferroic or linear magnetoelectric substitution series [(NH 4) 1−x K x ] 2 [FeCl 5 (H 2 O)]. Pyroelectric currents, magnetic susceptibilities, and thermodynamic properties were examined on large single crystals of the erythrosiderite compounds and detailed magnetic-field versus temperature phase diagrams are derived for three different substitution levels. With increasing potassium concentration the material is tuned from a multiferroic (x 0.06) to a linear magnetoelectric (x 0.15) ground state. In contrast to the respective pure parent compounds with x = 0 or 1, however, the ferroelectric or linear magnetoelectric polarization in none of the substituted samples is switchable by external electric fields because these samples exhibit a significant electric polarization already above the magnetic ordering transition. The polarization arises at a higher-lying structural phase transition that is examined by THz spectroscopy, and, on a deuterated pure single crystal, by comprehensive neutron-diffraction experiments. The structural phase transition is attributed to an ordering of NH + 4 tetrahedra but does not break inversion symmetry in the pure material, while a finite K content causes pyroelectricity.

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“…Ferroelectricity below 6.9 K is attributed to the inverse Dzyaloshinskii-Moriya (DM) mechanism, which predicts that the electric polarization is proportional to (S i × S j ) × Q, leading to an electric polarization along the a-axis [24]. These properties have been extensively discussed in previous inelastic neutron scattering experiments [25] and theoretical studies based on density functional theory (DFT) [26] and spin models [27].…”

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confidence: 99%

Phase transitions of the ferroelectric $(\mathrm{ND}_4)_2\mathrm{FeCl}_5\cdot\mathrm{D}_2\mathrm{O}$ under a magnetic field

Li,

Fishman

2021

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Due to the strong coupling between magnetism and ferroelectricity, (ND4)2FeCl5 • D2O exhibits several intriguing magnetic and electric phases. In this letter, we include high-order onsite spin anisotropic interactions in a spin model that successfully captures the ferroelectric phase transitions of (ND4)2FeCl5 • D2O under a magnetic field and produces the large weights of high-order harmonic components in the cycloid structure that are observed from neutron diffraction experiments. Moreover, we predict a new ferroelectric phase sandwiched between the FE II and FE III phases in a magnetic field. Our results emphasize the importance of the high-order spin anisotropic interactions and provide a guideline to understand multiferroic materials with rich phase diagrams.

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Magnetic field-temperature phase diagram of multiferroic (NH4)2FeCl5·H2O

Cited by 16 publications

References 66 publications

Magnetoelectric coupling in the mixed erythrosiderite [(NH4)1−xKx]<

Magnetoelectric coupling in the mixed erythrosiderite [(NH4)1−xKx]<

Domain switching and exchange bias control by electric field in the multiferroic conical magnet Mn2GeO4

Phase transitions of the ferroelectric $(\mathrm{ND}_4)_2\mathrm{FeCl}_5\cdot\mathrm{D}_2\mathrm{O}$ under a magnetic field

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