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Charge order, dynamics, and magneto-structural transition in multiferroic LuFe$_2$O$_4$

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 Added by Xiaoshan Xu
 Publication date 2008
  fields Physics
and research's language is English




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We investigated the series of temperature and field-driven transitions in LuFe$_2$O$_4$ by optical and M{o}ssbauer spectroscopies, magnetization, and x-ray scattering in order to understand the interplay between charge, structure, and magnetism in this multiferroic material. We demonstrate that charge fluctuation has an onset well below the charge ordering transition, supporting the order by fluctuation mechanism for the development of charge order superstructure. Bragg splitting and large magneto optical contrast suggest a low temperature monoclinic distortion that can be driven by both temperature and magnetic field.



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Using neutron diffraction, we have studied the magnetic field effect on charge structures in the charge-ordered multiferroic material LuFe$_2$O$_4$. An external magnetic field is able to change the magnitude and correlation lengths of the charge valence order even before the magnetic order sets in. This affects the dielectric and ferroelectric properties of the material and induces a giant magneto-electric effect. Our results suggest that the magneto-electric coupling in LuFe$_2$O$_4$ is likely due to magnetic field effect on local spins, in clear contrast to the case in most other known multiferroic systems where the bulk magnetic order is important.
The reflectivity of a large LuFe(2)O(4) single crystal has been measured with the radiation field either perpendicular or parallel to the c axis of its rhombohedral structure, from 10 to 500K, and from 7 to 16000 cm-1. The transition between the two-dimensional and the three-dimensional charge order at T_(CO) = 320 K is found to change dramatically the phonon spectrum in both polarizations. The number of the observed modes above and below T_(CO), according to a factor-group analysis, is in good agreement with a transition from the rhombohedral space group R{bar 3}m to the monoclinic C2/m. In the sub-THz region a peak becomes evident at low temperature, whose origin is discussed in relation with previous experiments.
We performed elastic neutron scattering measurements on the charge- and magnetically-ordered multiferroic material LuFe(2)O(4). An external electric field along the [001] direction with strength up to 20 kV/cm applied at low temperature (~100 K) does not affect either the charge or magnetic structure. At higher temperatures (~360 K), before the transition to three-dimensional charge-ordered state, the resistivity of the sample is low, and an electric current was applied instead. A reduction of the charge and magnetic peak intensities occurs when the sample is cooled under a constant electric current. However, after calibrating the real sample temperature using its own resistance-temperature curve, we show that the actual sample temperature is higher than the thermometer readings, and the intensity reduction is entirely due to internal sample heating by the applied current. Our results suggest that the charge and magnetic orders in LuFe(2)O(4) are unaffected by the application of external electric field/current, and previously observed electric field/current effects can be naturally explained by internal sample heating.
We investigate the crystal structure and lattice vibrations of Sr$_2$IrO$_4$ by a combined phonon Raman scattering and x-ray powder diffraction experiment under pressures up to $66$ GPa and room temperature. Density functional theory (DFT) and $ab$-initio lattice dynamics calculations were also carried out. A first-order structural phase transition associated with an $8$ % collapse of the $c$-axis is observed at high pressures, with phase coexistence being observed between $sim 40$ and $55$ GPa. At lower pressures, lattice and phonon anomalies were observed, reflecting crossovers between isostructural competing states. A critical pressure of $P_1=17$ GPa is associated with: (i) a reduction of lattice volume compressibility and a change of behavior of the tetragonal $c/a$ ratio take place above $P_1$; (ii) a four-fold symmetry-breaking lattice strain associated with lattice disorder; (iii) disappearance of two Raman active modes (at $sim 180$ and $sim 260$ cm$^{-1}$); and (iv) development of an asymmetric Fano lineshape for the $sim 390$ cm$^{-1}$ mode. DFT indicates that the phase above $P_1$ is most likely non-magnetic. Exploring the similarities between iridate and cuprate physics, we argue that these observations are consistent with the emergence of a rotational symmetry-breaking electronic instability at $P_1$, providing hints for the avoided metallization under pressure and supporting the hypothesis of possible competing orders that are detrimental to superconductivity in this family. Alternative scenarios for the transition at $P_1$ are also suggested and critically discussed. Additional phonon and lattice anomalies in the tetragonal phase are observed at $P_2=30$ and $P_3=40$ GPa, indicating further competing phases that are stabilized at high pressures.
The magnetic structure and the multiferroic relaxation dynamics of NaFeGe$_2$O$_6$ were studied by neutron scattering on single crystals partially utilizing polarization analysis. In addition to the previously reported transitions, the incommensurate spiral ordering of Fe$^{3+}$ moments in the $ac$ plane develops an additional component along the crystallographic $b$ direction below $Tapprox 5text{ K}$, which coincides with a lock-in of the incommensurate modulation. The quasistatic control of the spin-spiral handedness, respectively of the vector chirality, by external electric fields proves the invertibility of multiferroic domains down to the lowest temperature. Time-resolved measurements of the multiferroic domain inversion in NaFeGe$_2$O$_6$ reveal a simple temperature and electric-field dependence of the multiferroic relaxation that is well described by a combined Arrhenius-Merz relation, as it has been observed for TbMnO$_3$. The maximum speed of domain wall motion is comparable to the spin wave velocity.
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