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Register a new userSymmetry Analysis of Magnetoelectric Effects in Honeycomb Antiferromagnet Co4Nb2O9
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Added by
Masashige Matsumoto
Publication date
2019
fields
Physics
and research's language is
English
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Magnetoelectric effects in honeycomb antiferromagnet Co4Nb2O9 are investigated on the basis of symmetry analyses of Co ions in trigonal P-3c1 space group. For each Co ion, the possible spin dependence is classified by C3 point-group symmetry. This accounts for the observed main effect that an electric polarization rotates in the opposite direction at the twice speed relative to the rotation of the external magnetic field applied in the ab-plane. Inversion centers and twofold axes in the unit cell restrict the active spin-dependence of the electric polarization, which well explains the observed experimental results. Expected optical properties of quadrupolar excitation and various types of dichroism are also discussed.
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The honeycomb antiferromagnet Co4Nb2O9 is known to exhibit an interesting magnetoelectric effect that the electric polarization rotates at the twice speed in the opposite direction relative to the rotation of the external magnetic field applied in the basal ab-plane. The spin-dependent electric dipole can be an origin of the magnetoelectric effect. It is described by the product of spin operators at different sites (type-I theory) or at the same site (type-II theory). We examine the electric polarization for the two cases on the basis of the symmetry analysis of the crystal structure of Co4Nb2O9, and conclude that the latter is the origin of the observed result. This paper also gives a general description of the field-induced electric polarization on honeycomb lattices with the C3 point group symmetry on the basis of the type-I theory.
Spin-dependent electric dipole operators are investigated group-theoretically for the emergence of an electric dipole induced by a single spin or by two spins, where the spin dependences are completely classified up to the quadratic order. For a single spin, a product of spin operators behaves as an even-parity electric quadrupole operator, which differs from an odd-parity electric dipole. The lack of the inversion symmetry allows the even- and odd-parity mixing, which leads to the electric dipole described by the electric quadruple operators. Point-group tables are given for classification of the possible spin-dependent electric dipoles and for the qualitative analysis of multiferroic properties, such as an emergent electric dipole moment coexisting with a magnetic moment, electromagnon excitation, and directional dichroism. The results can be applied to a magnetic ion in crystals or embedded in molecules at a site without the inversion symmetry. In the presence of an inversion symmetry, the electric dipole does not appear for a single spin. This is not the case for the electric dipole induced by two spins with antisymmetric spin dependence, which is known as vector spin chirality, in the presence of the inversion center between the two spins. In the absence of the inversion center, symmetric spin-dependent electric dipoles are also relevant. The detailed analysis of various symmetries of two-spin states is applied to spin dimer systems and the related multiferroic properties.
We obtain the most general forms of rank-2 and rank-3 tensors allowed by the crystal symmetries of the honeycomb lattice of edge-sharing octahedra for crystals belonging to different crystallographic point groups, including the monoclinic point group $2/m$ and the trigonal (or rhombohedral) point group $bar{3}$. Our results are relevant for two-dimensional materials, such as $alpha$-RuCl$_3$, CrI$_3$, and the honeycomb iridates. We focus on the magnetic-field-dependent thermal conductivity tensor $kappa_{ij}(mathbf{H})$, which describes a systems longitudinal and thermal Hall responses, for the cases when the magnetic field is applied along high-symmetry directions, perpendicular to the plane and in the plane. We highlight some unexpected results, such as the equality of fully-longitudinal components to partially-transverse components in rank-3 tensors for systems with three-fold rotational symmetry, and make testable predictions for the thermal conductivity tensor.
The magnetic and magnetocaloric (MCE) properties were studied in a stuffed honeycomb antiferromagnet GdInO3 polycrystalline. No long-range magnetic ordering was observed with only a sharp upturn in the temperature dependent magnetization curves at TN ~ 2.1 K. The large value of frustration index value ~ 5.0 suggests short-range antiferromagnetic interactions existing between the Gd3+ moments in this frustrated magnetic system. Negligible thermal and magnetic hysteresis suggest a second-order feature of phase transition and a reversible magnetocaloric effect (MCE) in GdInO3 compound. In the magnetic field changes of 0-50 kOe and 0-70 kOe, the maximum magnetic entropy change values are 9.31 J/kg K and 17.53 J/kg K near the liquid helium temperature, with the corresponding RCP values of 106.61 and 196.38 J/kg, respectively. The relative lower MCE performance of GdInO3 polycrystalline than the other Gd-based magnetocaloric effect is understood by the high magnetic frustration in this system. Our investigation results reveal GdInO3 polycrystalline has a large reversible MCE, which not only provides another possibility of exploiting magnetocaloric refrigerants in the frustrated magnetic systems near the cryogenic temperature region, but also serves to excavate more exotic properties in the frustrated stuffed honeycomb magnetic systems.
By combining single crystal x-ray and neutron diffraction, and the magnetodielectric measurements on single crystal Fe4Nb2O9, we present the magnetic structure and the symmetry-allowed magnetoelectric coupling in Fe4Nb2O9. It undergoes an antiferromagnetic transition at TN=93 K, followed by a displacive transition at TS=70 K. The temperature-dependent dielectric constant of Fe4Nb2O9 is strongly anisotropic with the first anomaly at 93 K due to the exchange striction as a result of the long range spin order, and the second one at 70 K emanating from the structural phase transition primarily driven by the O atomic displacements. Magneticfield induced magnetoelectric coupling was observed in single crystal Fe4Nb2O9 and is compatible with the solved magnetic structure that is characteristic of antiferromagnetically arranged ferromagnetic chains in the honeycomb plane. We propose that such magnetic symmetry should be immune to external magnetic fields to some extent favored by the freedom of rotation of moments in the honeycomb plane, laying out a promising system to control the magnetoelectric properties by magnetic fields.
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