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Register a new userSpin structure and magnetic frustration in multiferroic RMn2O5 (R = Tb, Ho, Dy)
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G.R. Blake
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We have studied the crystal and magnetic structures of the magnetoelectric materials RMn2O5 (R = Tb, Ho, Dy) using neutron diffraction as a function of temperature. All three materials display incommensurate antiferromagnetic ordering below 40 K, becoming commensurate on further cooling. For R = Tb, Ho, a commensurate-incommensurate transition takes place at low temperatures. The commensurate magnetic structures have been solved and are discussed in terms of competing exchange interactions. The spin configuration within the ab plane is essentially the same for each system, and the radius of R determines the sign of the magnetic exchange between adjacent planes. The inherent magnetic frustration in these materials is lifted by a small lattice distortion, primarily involving shifts of the Mn3+ cations and giving rise to a canted antiferroelectric phase.
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Measurements of ferroelectric polarization and dielectric constant were done on $R$Mn$_2$O$_5$ ($R$=Tb, Dy, and Ho) with applied hydrostatic pressures of up to 18 kbar. At ambient pressure, distinctive anomalies were observed in the temperature profile of both physical properties at critical temperatures marking the onset of long range AFM order (T$_{N1}$), ferroelectricity (T$_{C1}$) as well as at temperatures when anomalous changes in the polarization, dielectric constant and spin wave commensurability have been previously reported. In particular, the step in the dielectric constant at low temperatures (T$_{C2}$), associated with both a drop in the ferroelectric polarization and an incommensurate magnetic structure, was shown to be suddenly quenched upon passing an $R$-dependent critical pressure. This was shown to correlate with the stabilization of the high ferroelectric polarization state which is coincident with the commensurate magnetic structure. The observation is suggested to be due to a pressure induced phase transition into a commensurate magnetic structure as exemplified by the pressure-temperature ($p$-$T$) phase diagrams constructed in this work. The $p$-$T$ phase diagrams are determined for all three compounds.
We investigated the effects of temperature and magnetic field on the electronic structure of hexagonal RMnO3 (R = Gd, Tb, Dy, and Ho) thin films using optical spectroscopy. As the magnetic ordering of the system was disturbed, a systematic change in the electronic structure was commonly identified in this series. The optical absorption peak near 1.7 eV showed an unexpectedly large shift of more than 150 meV from 300 K to 15 K, accompanied by an anomaly of the shift at the Neel temperature. The magnetic field dependent measurement clearly revealed a sizable shift of the corresponding peak when a high magnetic field was applied. Our findings indicated strong coupling between the magnetic ordering and the electronic structure in the multiferroic hexagonal RMnO3 compounds.
We have used a shell model to study the phonon dynamics of multiferroic manganites RMnO3 (R= Tb, Dy, Ho). The calculated phonon dynamical properties, crystal structure, Raman frequencies and specific heat are found to be in good agreement with the available experimental data. Besides, the phonon density of states, elastic constants and phonon dispersion curves along high symmetry directions (sigma, delta and lambda) have also been computed. A zone-center imaginary Au mode is revealed in these phonon dispersion curves, which indicates the occurrence of metastability of the perovskite phase. The Gibbs free energy values of orthorhombic phase, when compared with those of hexagonal phase, indicate the possibility of coexistence of these two phases of these multiferroic manganites under ambient conditions.
We investigated the electronic structure of multiferroic hexagonal RMnO3 (R = Gd, Tb, Dy, and Ho) thin films using both optical spectroscopy and first-principles calculations. Using artificially stabilized hexagonal RMnO3, we extended the optical spectroscopic studies on the hexagonal multiferroic manganite system. We observed two optical transitions located near 1.7 eV and 2.3 eV, in addition to the predominant absorption above 5 eV. With the help of first-principles calculations, we attribute the low-lying optical absorption peaks to inter-site transitions from the oxygen states hybridized strongly with different Mn orbital symmetries to the Mn 3d3z2-r2 state. As the ionic radius of the rare earth ion increased, the lowest peak showed a systematic increase in its peak position. We explained this systematic change in terms of a flattening of the MnO5 triangular bipyramid.
The magnetic structures of the title compounds have been studied by neutron diffraction. In contrast to the isomorphous RNi2B2C compounds wherein a variety of exotic incommensurate modulated structures has been observed, the magnetic structure of ErCo2B2C is found to be collinear antiferromagnet with k=((1/2),0,(1/2)) while that of HoCo2B2C and DyCo2B2C are observed to be simple ferromagnets. For all studied compounds, the moments are found to be confined within the basal plane and their magnitudes are in good agreement with the values obtained from the low-temperature isothermal magnetization measurements. The absence of modulated magnetic structures in the RCo2B2C series (for ErCo2B2C, verified down to 50 mK) is attributed to the quenching of the Fermi surface nesting features.
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