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Register a new userObservation of an inter-sublattice exchange magnon in CoCr$_2$O$_4$ and analysis of magnetic ordering
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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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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$_4$.
Bulk magnetic, X-ray and neutron diffraction measurements were performed on polycrystalline Tb14Ag51 in the temperature range from 1.5 K to room temperature. Its chemical Gd14Ag51 type structure corresponds to space group P6/m. Combined with group theoretical symmetry analysis, we show that the magnetic structure of this intermetallic compound is of a new k = (1/3,1/3,0) type with three magnetic Tb sublattices ordering simultaneously below TN = 27.5(5) K according to the combined irreducible representations tau4 and tau6. Here we present a general analysis of possible magnetic A ordering for k = (1/3,1/3,0) in A14B51 compounds.
The magnetic properties of the cobaltite {BCAO}, a good realization of the quasi two-dimensional frustrated honeycomb-lattice system with strong planar anisotropy, have been reinvestigated by means of spherical neutron polarimetry with CRYOPAD. From accurate measurements of polarization matrices both on elastic and inelastic contributions as a function of the scattering vector {bf{Q}}, we have been able to determine the low-temperature magnetic structure of {BCAO} and reveal its puzzling in-plane spin dynamics. Surprisingly, the ground-state structure (described by an incommensurate propagation vector ${bf{k}}_{1}=(k_{x}, 0, k_{z}$), with $k_{x}=0.270{pm}0.005$ and $k_{z} approx -1.31$) appears to be a quasi-collinear structure, and not a simple helix, as previously determined. In addition, our results have revealed the existence of a non-negligible out-of-plane moment component $ approx 0.25{mu}_{B}$/Co$^{2+}$, representing about 10% of the in-plane component, as demonstrated by the presence of finite off-diagonal elements $P_{yz}$ and $P_{zy}$ of the polarization matrix, both on elastic and inelastic magnetic contributions. Despite a clear evidence of the existence of a slightly inelastic contribution of structural origin superimposed to the magnetic excitations at the scattering vectors ${bf{Q}}=(0.27, 0, 3.1)$ and ${bf{Q}}=(0.73, 0, 0.8)$ (energy transfer ${Delta}E approx 2.3$ meV), no strong inelastic nuclear-magnetic interference terms could be detected so far, meaning that the nuclear and magnetic degrees of freedom have very weak cross-correlations. The strong inelastic $P_{yz}$ and $P_{zy}$ matrix elements can be understood by assuming that the magnetic excitations in {BCAO} are spin waves associated with trivial anisotropic precessions of the magnetic moments involved in the canted incommensurate structure.
Using realistic low-energy model with parameters derived from the first-principles electronic structure calculation, we address the origin of the quasi-one-dimensional behavior in orthorhombic NaV$_2$O$_4$, consisting of the double chains of edge-sharing VO$_6$ octahedra. We argue that the geometrical aspect alone does not explain the experimentally observed anisotropy of electronic and magnetic properties of NaV$_2$O$_4$. Instead, we attribute the unique behavior of NaV$_2$O$_4$ to one particular type of the orbital ordering, which respects the orthorhombic $Pnma$ symmetry. This orbital ordering acts to divide all $t_{2g}$ states into two types: the `localized ones, which are antisymmetric with respect to the mirror reflection $y rightarrow -$$y$, and the symmetric `delocalized ones. Thus, NaV$_2$O$_4$ can be classified as the double exchange system. The directional orientation of symmetric orbitals, which form the metallic band, appears to be sufficient to explain both quasi-one-dimensional character of interatomic magnetic interactions and the anisotropy of electrical resistivity.
We study the exchange constants of MnV$_2$O$_4$ using magnetic force theorem and local spin density approximation of density functional theory supplemented with a correction due to on-site Hubbard interaction U. We obtain the exchanges for three different orbital orderings of the Vanadium atoms of the spinel. We then map the exchange constants to a Heisenberg model with single-ion anisotropy and solve for the spin-wave excitations in the non-collinear, low temperature phase of the spinel. The single-ion anisotropy parameters are obtained from an atomic multiplet exact-diagonalization program, taking into effect the crystal-field splitting and the spin-orbit coupling. We find good agreement between the spin waves of one of our orbital ordered setups with previously reported experimental spin waves as determined by neutron scattering. We can therefore determine the correct orbital order from various proposals that exist in the literature.
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