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Spin Dynamics and Magnetoelectric Coupling Mechanism of Co4Nb2O9

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 Added by Guochu Deng
 Publication date 2017
  fields Physics
and research's language is English




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Neutron powder diffraction experiments reveal that Co4Nb2O9 forms a noncollinear in-plane magnetic structure with Co2+ moments lying in the ab plane. The spin-wave excitations of this magnet were measured by using inelastic neutron scattering and soundly simulated by a dynamic model involving nearest and next-nearest neighbour exchange interactions, in-plane anisotropy and the Dzyaloshinskii-Moriya interaction. The in-plane magnetic structure of Co4Nb2O9 is attributed to the large in-plane anisotropy while the noncollinearity of the spin configuration is attributed to the Dzyaloshinskii-Moriya interaction. The high magnetoelectric coupling effect of Co4Nb2O9 in fields can be explained by its special in-plane magnetic structure.



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Co4Nb2O9 (CNO) having {alpha}-Al2O3 crystal structure with Co chains along c-direction shows gigantic magnetoelelctric coupling below antiferromagnetic ordering temperature of 27 K but above a spin flop field of 1.6 T. We have investigated structural, magnetic and magnetoelectric properties of Fe substituted (10% and 20%) samples and compared with the parent one. In fact magnetic and specific heat measurements have revealed an additional magnetic transition below 10 K and presence of short range magnetic ordering above ~ 50 K in parent as well as in Fe substituted samples. Linear magnetoelelctric and ferroelectric behaviours are evidenced in the Fe substituted samples where an electric field of 5 kV/m is sufficient to align the dipoles and the magnetoelelctric coupling is ensured for magnetic fields as low as 0.25 T, far below the spin flop field.
Synthesis and extensive structural, pyroelectric, magnetic, dielectric and magneto-electric characterizations are reported for polycrystalline Co4Nb2O9 towards unraveling the multiferroic state especially in reference to the magnetic spin flop transition. Magnetic measurements confirm the Co4Nb2O9 becomes antiferromagnetic (AFM) at around 28 K but no clear evidence for spin-flop effect was found. Associated with the magnetic phase transition, a sharp peak in pyroelectric current indicates the appearance of the strong magneto-electric coupling below Neel temperature (TN) with a large coupling constant upto 17.8 uC/m^2T. Using temperature oscillation technique, we establish Co4Nb2O9 to be a genuine multiferroic with spontaneous electric polarization in the anti-ferromagnetic state.
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.
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.
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