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Temperature- and Magnetic-Field-Tuning of Magnetic Phases in Multiferroic NdFe3(BO3)4

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 Added by Christie S. Nelson
 Publication date 2013
  fields Physics
and research's language is English




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We report the low-temperature coexistence in NdFe3(BO3)4 of an incommensurate magnetic phase with a strained commensurate magnetic phase that is primarily at the surface of the crystal. Increasing the temperature or magnetic field decreases the incommensurability and stabilizes the commensurate magnetic phase above Tic ~14 K or Hic = 0.9 T. A comparison to published studies indicates the onset of longitudinal magnetostriction and electric polarization at the magnetic-field-induced transition, which may arise due to a basal plane spin-flop and canting of the moments along the field direction.



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Complex experimental and theoretical study of the magnetic, magnetoelectric, and magnetoelastic properties of neodymium iron borate NdFe3(BO3)4 along various crystallographic directions have been carried out in strong pulsed magnetic fields up to 230 kOe in a temperature range of 4.2-50 K. It has been found that neodymium iron borate, as well as gadolinium iron borate, is a multiferroic. It has much larger (above 3 10^(-4) C/m^2) electric polarization controlled by the magnetic field and giant quadratic magnetoelectric effect. The exchange field between the rare-earth and iron subsystems (~50 kOe) has been determined for the first time from experimental data. The theoretical analysis based on the magnetic symmetry and quantum properties of the Nd ion in the crystal provides an explanation of an unusual behavior of the magnetoelectric and magnetoelastic properties of neodymium iron borate in strong magnetic fields and correlation observed between them.
We report high-resolution optical absorption spectra for NdFe3(BO3)4 trigonal single crystal which is known to exhibit a giant magnetoelectric effect below the temperature of magnetic ordering TN = 33 K. The analysis of the temperature-dependent polarized spectra reveals the energies and, in some cases, symmetries and exchange splittings of Nd3+ 84 Kramers doublets. We perform crystal-field calculations starting from the exchange-charge model, obtain a set of six real crystal-field parameters, and calculate wave functions and magnetic g-factors. In particular, the values g(perpendicular) = 2.385, g(parallel) = 1.376 were found for the Nd3+ ground-state doublet. We obtain Bloc=7.88 T and |JFN|= 0.48 K for the values of the local effective magnetic field at liquid helium temperatures at the Nd3+ site and the Nd - Fe exchange integral, respectively, using the experimentally measured Nd3+ ground-state splitting of 8.8 cm-1. To check reliability of our set of crystal field parameters we model the magnetic susceptibility data from literature. A dimer containing two nearest-neighbor iron ions in the spiral chain is considered to partly account for quasi-one-dimensional properties of iron borates, and then the mean-field approximation is used. The results of calculations with the exchange parameters for Fe3+ ions Jnn = -6.25 K (intra-chain interactions) and Jnnn = -1.92 K (inter-chain interactions) obtained from fitting agree well with the experimental data.
We report a magnetic x-ray scattering study of the field-induced multiferroic GdFe3(BO3)4. Resonant x-ray magnetic scattering at the Gd LII,III edges indicates that the Gd moments order at TN ~ 37 K. The magnetic structure is incommensurate below TN, with the incommensurability decreasing monotonically with decreasing temperature until a transition to a commensurate magnetic phase is observed at T ~ 10 K. Both the Gd and Fe moments undergo a spin reorientation transition at TSR ~ 9 K such that the moments are oriented along the crystallographic c axis at low temperatures. With magnetic field applied along the a axis, our measurements suggest that the field-induced polarization phase has a commensurate magnetic structure with Gd moments rotated ~45 degrees toward the basal plane, which is similar to the magnetic structure of the Gd subsystem observed in zero field between 9 and 10 K, and the Fe subsystem has a ferromagnetic component in the basal plane.
Resonant and non-resonant X-ray scattering studies on HoFe3(BO3)O4 reveal competing magnetic ordering of Ho and Fe moments. Temperature and X-ray polarization dependent measurements employed at the Ho L3 edge directly reveal a spiral spin order of the induced Ho moments in the ab-plane propagating along the c-axis, a screw-type magnetic structure. At about 22.5 K the Fe spins are observed to rotate within the basal plane inducing spontaneous electric polarization, P. Components of P in the basal plane and along the c-axis can be scaled with the separated magnetic X-ray scattering intensities of the Fe and Ho magnetic sublattices, respectively.
The structural phase transition in hexagonal BaMnO$_3$ occurring at $T_c$=130 K was studied in ceramic samples using electron and X-ray diffraction, second harmonic generation as well as by dielectric and lattice dynamic spectroscopies. The low-temperature phase (space group $P6_{3}cm$) is ferroelectric with a triplicated unit cell. The phase transition is driven by an optical soft mode from the Brillouin-zone boundary [$q = (frac{1}{3},frac{1}{3},0)$]; this mode activates in infrared and Raman spectra below $T_c$ and it hardens according to the Cochran law. Upon cooling below $T_c$, the permittivity exhibits an unusual linear increase with temperature; below 60 K, in turn, a frequency-dependent decrease is observed, which can be explained by slowing-down of ferroelectric domain wall motions. Based on our data we could not distinguish whether the high-temperature phase is paraelectric or polar (space groups $P6_{3}/mmc$ or $P6_{3}mc$, respectively). Both variants of the phase transition to the ferroelectric phase are discussed based on the Landau theory. Electron paramagnetic resonance and magnetic susceptibility measurements reveal an onset of one-dimensional antiferromagnetic ordering below $approx220,rm K$ which develops fully near 140 K and, below $T_{n} approx 59,rm K$, it transforms into a three-dimensional antiferromagnetic order.
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