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Magnetic ordering and magnetodielectric phenomena in CoSeO$_4$

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 Added by Brent Melot
 Publication date 2010
  fields Physics
and research's language is English




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CoSeO$_4$ has a structure consisting of edge-sharing chains of Co$^{2+}$ octahedra which are held together by SeO$_4^{2-}$ tetrahedra via shared oxygen atoms at the edges of the octahedra. DC magnetization measurements indicate a transition to an ordered state below 30 K. Powder neutron diffraction refinements suggest an ordered state with two unique antiferrromagnetic chains within the unit cell. Isothermal magnetization measurements indicate a temperature-dependent field-induced magnetic transition below the ordering temperature. From neutron diffraction, we find this corresponds to a realignment of spins from the canted configuration towards the c-axis. The dielectric constant shows a change in slope at the magnetic ordering temperature as well as a quadratic dependence on the external magnetic field.



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Magnetoelectric materials have generated wide technological and scientific interest because of the rich phenomena these materials exhibit, including the coexistence of magnetic and ferroelectric orders, magnetodielectric behavior, and exotic hybrid excitations such as electromagnons. The multiferroic spinel material, CoCr$_2$O$_4$, is a particularly interesting example of a multiferroic material, because evidence for magnetoelectric behavior in the ferrimagnetic phase seems to conflict with traditional noncollinear-spin-driven mechanisms for inducing a macroscopic polarization. This paper reports an inelastic light scattering study of the magnon and phonon spectrum of CoCr$_2$O$_4$ as simultaneous functions of temperature, pressure, and magnetic field. Below the Curie temperature ($T_C sim 94$ K) of CoCr$_2$O$_4$ we observe a $omega sim 16 ,text{cm}^{-1}$ $boldsymbol q=0$ magnon having T$_{1g}$-symmetry, which has the transformation properties of an axial vector. The anomalously large Raman intensity of the T$_{1g}$-symmetry magnon is characteristic of materials with a large magneto-optical response and likely arises from large magnetic fluctuations that strongly modulate the dielectric response in CoCr$_2$O$_4$. The Raman susceptibility of the T$_{1g}$-symmetry magnon exhibits a strong magnetic-field dependence that is consistent with the magnetodielectric response observed in CoCr$_2$O$_4$, suggesting that magnetodielectric behavior in CoCr$_2$O$_4$ primarily arises from the field-dependent suppression of magnetic fluctuations that are strongly coupled to long-wavelength phonons. Increasing the magnetic anisotropy in CoCr$_2$O$_4$ with applied pressure decreases the magnetic field-dependence of the T$_{1g}$-symmetry magnon Raman susceptibility in CoCr$_2$O$_4$, suggesting that strain can be used to control the magnetodielectric response in CoCr$_2$O$_4$.
We have carried out dc magnetization (M), heat-capacity (C) and dielectric studies down to 2K for the compound GdCrTiO5, crystallizing in orthorhombic Pbam structure, in which well-known multiferroics RMn2O5 (R= Rare-earths) form. The points of emphasis are: (i) The magnetic ordering temperature of Cr appears to be suppressed compared to that in isostructural Nd counterpart, NdCrTiO5, for which the Neel temperature is about 21 K. This finding on the Gd compound suggests that Nd 4f orbital plays a role on the magnetism of Cr in contrast to a proposal long ago. (ii) Dielectric constant does not exhibit any notable feature below about 30 K in the absence of external magnetic field, but a peak appears and gets stronger with the application of external magnetic fields, supporting the existence of magnetodielectric coupling. (iii) The dielectric anomalies appear even near 100 K, which can be attributed to short-range magnetic-order. We also observe a gain in spectral weight below about 150 K in Raman spectra in the frequency range 150 to 400 cm-1, which could be magnetic in origin supporting short-range magnetic order. It is of interest to explore whether geometrically frustration plays any role on the dielectric properties of this family, as in the case of RMn2O5.
Orthorhombic HoMnO3 is a multiferroic in which Mn antiferromagnetic order induces ferroelectricity. A second transition occurs within the multiferroic phase, in which a strong enhancement of the ferroelectric polarization occurs concomitantly to antiferromagnetic ordering of Ho 4f magnetic moments. Using the element selectivity of resonant X-ray diffraction, we study the magnetic order of the Mn 3d and Ho 4f moments. We explicitly show that the Mn magnetic order is affected by the Ho 4f magnetic ordering transition. Based on the azimuthal dependence of the (0 q 0) and (0 1-q 0) magnetic reflections, we suggest that the Ho 4f order is similar to that previously observed for Tb 4f in TbMnO3, which resembles an ac-cycloid. This is unlike the Mn order, which has already been shown to be different for the two materials. Using non-resonant diffraction, we show that the magnetically-induced ferroelectric lattice distortion is unaffected by the Ho ordering, suggesting a mechanism through which the Ho order affects polarization without affecting the lattice in the same manner as the Mn order.
We report the magnetic, heat-capacity, dielectric and magnetodielectric (MDE) behaviour of a Haldane spin-chain compound containing light rare-earth ion, Nd2BaNiO5, in detail, as a function of temperature (T) and magnetic field (H) down to 2 K. In addition to the well-known long range antiferromagnetic order setting in at (T_N=) 48 K as indicated in dc magnetization (M), we have observed another magnetic transition near 10 K; this transition appears to be of a glassy-type which vanishes with a marginal application of external magnetic field (even H= 100 Oe). There are corresponding anomalies in dielectric constant as well with variation of T. The isothermal M(H) curves at 2 and 5 K reveal the existence of a magnetic-field induced transition around 90 kOe; the isothermal H-dependent dielectric constant also tracks such a metamagnetic transition. These results illustrate the MDE coupling in this compound. Additionally, we observe a strong frequency dependence of a step in T-dependent dielectric constant with this feature appearing around 25-30 K for the lowest frequency of 1 kHz, far below T_N. This is attributed to interplay between crystal-field effect and exchange interaction between Nd and Ni, which establishes the sensitivity of dielectric measurements to detect such effects. Interestingly enough, the observed dispersions of the T-dependent dielectric constant curves is essentially H-independent in the entire T-range of measurement, despite the existence of MDE coupling, which is in sharp contrast with other heavy rare-earth members in this series.
We report on an investigation of optical properties of multiferroic CoCr$_{2}$O$_{4}$ at terahertz frequencies in magnetic fields up to 30 T. Below the ferrimagnetic transition (94 K), the terahertz response of CoCr$_{2}$O$_{4}$ is dominated by a magnon mode, which shows a steep magnetic-field dependence. We ascribe this mode to an exchange resonance between two magnetic sublattices with different $g$-factors. In the framework of a simple two-sublattice model (the sublattices are formed by Co$^{2+}$ and Cr$^{3+}$ ions), we find the inter-sublattice coupling constant, $lambda = - (18 pm 1)$ K, and trace the magnetization for each sublattice as a function of field. We show that the Curie temperature of the Cr$^{3+}$ sublattice, $Theta_{2}$ = $(49 pm 2)$ K, coincides with the temperature range, where anomalies of the dielectric and magnetic properties of CoCr$_{2}$O$_{4}$ have been reported in literature.
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