Magnetically-induced ferroelectricity in the (ND4)2[FeCl5(D2O)] molecular compound

Rodríguez-Velamazán, J. A.; Fabelo, Óscar; Millán, Ángel; Campo, Javier; Johnson, Roger A.; Chapon, L. C.

doi:10.1038/srep14475

Cited by 37 publications

(70 citation statements)

References 41 publications

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“…This indicates a magnetic structure change from collinear sinusoidal to cycloidal spiral at T F E =6.8 K that suggests an inverse Dzyaloshinskii-Moriya mechanism for the induced ferroelectricity as proposed in Ref. 24. However, as we will show below, the cycloid structure is strongly distorted via spin-lattice coupling.…”

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confidence: 57%

Spin-lattice coupling mediated multiferroicity in (ND4)2FeCl5·D2O

Cao

Wang

et al. 2016

Phys. Rev. B

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We report a neutron diffraction study of the multiferroic mechanism in (ND4)2FeCl5•D2O, a molecular compound that exhibits magnetically induced ferroelectricity. This material exhibits two successive magnetic transitions on cooling: a long-range order transition to an incommensurate (IC) collinear sinusoidal spin state at TN =7.3 K, followed by a second transition to an IC cycloidal spin state at TF E =6.8 K, the later of which is accompanied by spontaneous ferroelectric polarization. The cycloid structure is strongly distorted by spin-lattice coupling as evidenced by the observations of both odd and even higher-order harmonics associated with the cycloid wave vector, and a weak commensurate phase that coexists with the IC phase. The appearance of the 2nd-order harmonic coincides with the onset of the electric polarization, thereby providing unambiguous evidence that the induced electric polarization is mediated by the spin-lattice interaction. Our results for this system, in which the orbital angular momentum is expected to be quenched, are remarkably similar to those of the prototypical TbMnO3, in which the magnetoelectric effect is attributed to spin-orbit coupling.

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confidence: 57%

Spin-lattice coupling mediated multiferroicity in (ND4)2FeCl5·D2O

Cao

Wang

et al. 2016

Phys. Rev. B

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“…Further microscopic and theoretical investigations are highly warranted to shade further light on magnetism, magnetodielectric coupling and possible ferroelectric order in this new class of MOFs. [34,37] To investigate the role of the polar nitrobenzene groups, we have performed magnetic and dielectric investigations on a MFU-2 compound, which has a similar structure without dipolar nitrobenzene groups. MFU-2 exhibits a similar magnetic ground state like CFA-12…”

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confidence: 99%

Magnetodielectric coupling in a non-perovskite metal–organic framework

et al. 2017

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Conceptual insightsSearch for magnetodielectric and multiferroic materials, in which magnetism can be tuned by electric fields, is of considerable interest not only for basic research but also for functionalities for future technological applications. One recent and very promising route is to search for such properties in metal-organic-frameworks (MOFs). However, until now, reports on multiferroicity in MOFs is restricted to a particular structure, so called perovskite structures, and also which mostly contain formate (HCOO) group responsible for mediating magnetic exchange interaction. Using the enormous flexibility (of ligand and guest molecules) of MOFs 2 system, we have designed a new MOF which crystallizes in a tetragonal structure and consists of Co spin chains, bridged by the functional ligand 4,4'-(2-nitrobenzol-1,4-diyl)bis (3,5-dimethyl-1H-pyrazol), containing a dipolar NO 2 group.Our result shows up that it might be possible to introduce cross-coupling between magnetism and dielectric even by simply introducing a dipolar group in a designed MOF in general, which opens up the possibility to design new MOFs in a wide variety of structure to achieve magnetodielectric coupling and multiferroicity. Therefore, our work yields a route to design new magnetodielectric MOFs which will help to achieve room temperature multiferroic for future potential applications in a long run. AbstractMultiferroicity and magnetodielectric coupling in metal-organic-frameworks (MOFs) is rare and so far restricted mainly to formate-based systems with perovskite structure. In the course of this work we designed a tetragonal framework [Co(C 16 H 15 N 5 O 2 )], exhibiting spinchains of Co 2+ ions, which are bridged by an organic linker containing a dipolar nitrobenzene moiety. This compound shows relaxor-like ferroelectricity at 100 K, which is followed by the onset of complex magnetic order at 15 K, indicative of weak ferromagnetism. The clear anomaly of the dielectric constant at the magnetic ordering transition indicates magnetodielectric coupling, which is also confirmed by magnetic-field dependent dielectric measurements. Weak ferromagnetism and magnetodielectric coupling, both probably result from a significant Dzyaloshinskii-Moriya interaction, which cants the spin structure and locally breaks inversion symmetry. We document that the introduction of dipolar nitrobenzene as building block in the crystal structure paths the way to design new multiferroic and magnetodielectric MOFs.

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“…A large single crystal of (ND 4 ) 2 [FeCl 5 (D 2 O)] of dimensions 5 x 3 x 2 mm along the crystallographic a-, b-and c-directions was obtained by the seeded growth technique as described in our previous work [26] . Neutron diffraction data were collected in the high resolution and low background D10 instrument at the Institut Laue-Langevin (Grenoble, France), operating in 'normal beam' geometry and equipped with a vertical-field cryomagnet, with selected applied magnetic fields ranging from 0 to 9.5 T along the a-and c-crystallographic directions.…”

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“…Based on the previous survey of the reciprocal space as a function of B, the magnetic structure in these phases is described using k 1 = (0, 0, ¼) and/or k 2 = (0, 0, 0) propagation vectors for 3.5 and 6 Tesla, respectively. Keeping the same nomenclature that in previous paper [26] , the four Fe(III) atoms in the primitive unit-cell labelled as Fe (1) can be calculated as:…”

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confidence: 99%

Magnetic-field-induced change of magnetoelectric coupling in the hybrid multiferroic (ND4)2[FeCl5·<

et al. 2017

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The possibility of cross-control of electric order by magnetic fields and magnetic order by electric fields is the key of the noticeable interest attracted by magneto-electric (ME) multiferroics, since it represents both a great potential for applications and a complex and fascinating topic for fundamental studies [1,2,3,4,5,6,7] . Two types of multiferroic materials are generally distinguished: "type I", where electric and magnetic orders coexist but are weakly coupled, and "type II", where electric polarization appears as a consequence of the magnetic ordering. In this last class, the competition between different magnetic exchange couplings often yields a complex ordered state that breaks inversion symmetry and induces ferroelectric polarization. This coupling scheme is realized through different mechanisms, which can be grouped into three major models: [8] (i) exchange striction, (ii) spin current, and (iii) spindependent p-d hybridization (which does not involve an exchange coupling but a single-ion term). For the exchange striction mechanism (i) to take place, a striction along a specific crystallographic axis may be induced by the symmetric exchange interaction between two neighboring spins, S i and S j , which couples to the pre-existing dipoles. Electric polarization, P, will be macroscopically observable if the induced striction is not cancelled after the sum over the bonds of the crystal lattice. This is the mechanism responsible for the induced polarization in compounds with collinear up-up-down-down spin structure ('E-type' antiferromagnetic structure) [9] . These compounds display the highest values of spin-driven ferroelectric polarization [10] . The spin current model (ii) is, in turn, probably the most thoroughly studied.This mechanism is responsible for the magneto-electric coupling in compounds with cycloidal spin arrangements such as RMnO 3 (R= rare earth) [11,12,13] MnWO 4 [14,15] or CoCr 2 O 4 [16] . According to this model, the antisymmetric Dzyaloshinskii-Moriya interactions [17,18] produce an

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Magnetically-induced ferroelectricity in the (ND4)2[FeCl5(D2O)] molecular compound

Cited by 37 publications

References 41 publications

Spin-lattice coupling mediated multiferroicity in (ND4)2FeCl5·D2O

Spin-lattice coupling mediated multiferroicity in (ND4)2FeCl5·D2O

Magnetodielectric coupling in a non-perovskite metal–organic framework

Magnetic-field-induced change of magnetoelectric coupling in the hybrid multiferroic (ND4)2[FeCl5·<

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