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Coupled magnetic and ferroelectric excitations in PbFe_{1/2}Nb_{1/2}O_{3}

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 Added by Chris Stock
 Publication date 2013
  fields Physics
and research's language is English




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A neutron scattering investigation of the magnetoelectric coupling in PbFe_{1/2}Nb_{1/2}O_{3} (PFN) has been undertaken. Ferroelectric order occurs below 400 K, as evidenced by the softening with temperature and subsequent recovery of the zone center transverse optic phonon mode energy (hbar Omega_{0}). Over the same temperature range, magnetic correlations become resolution limited on a terahertz energy scale. In contrast to the behavior of nonmagnetic disordered ferroelectrics (namely Pb(Mg,Zn)_{1/3}Nb_{2/3}O_{3}), we report the observation of a strong deviation from linearity in the temperature dependence of (hbar Omega_{0})^{2}. This deviation is compensated by a corresponding change in the energy scale of the magnetic excitations, as probed through the first moment of the inelastic response. The coupling between the short-range ferroelectric and antiferromagnetic correlations is consistent with calculations showing that the ferroelectricity is driven by the displacement of the body centered iron site, illustrating the multiferroic nature of magnetic lead based relaxors in the dynamical regime.



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We show that the magnetism of double perovskite AFe_{1/2}M_{1/2}O_3 systems may be described by the Heisenberg model on the simple cubic lattice, where only half of sites are occupied by localized magnetic moments. The nearest-neighbor interaction J_1 is more than 20 times the next-nearest neighbor interaction J_2, the third-nearest interaction along the space diagonal of the cube being negligible. We argue that the variety of magnetic properties observed in different systems is connected with the variety of chemical ordering in them. We analyze six possible types of the chemical ordering in 2x2x2 supercell, and argue that the probability to find them in a real compound does not correspond to a random occupation of lattice sites by magnetic ions. The exchange J_2 rather than J_1 define the magnetic energy scale of most double perovskite compounds that means the enhanced probability of 1:1 short range ordering. Two multiferroic compounds PbFe_{1/2}M_{1/2}O_3 (M=Nb, Ta) are exceptions. We show that the relatively high temperature of antiferromagnetic transition is compatible with a layered short-range chemical order, which was recently shown to be most stable for these two compounds [I. P. Raevski, {em et al.}, Phys. Rev. B textbf{85}, 224412 (2012)]. We show also that one of the types of ordering has ferrimagnetic ground state. The clusters with short-range order of this type may be responsible for a room-temperature superparamagnetism, and may form the cluster glass at low temperatures.
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Recently, materials exhibiting colossal dielectric constant ($CDC$) have attracted significant attention because of their high dielectric constant and potential applications in electronic devices, such as high dielectric capacitors, capacitor sensors, random access memories and so on.
We have characterized the dynamics of the polar nanoregions in Pb(Mg$_{1/3}$Nb$_{2/3}$)O$_{3}$ (PMN) through high-resolution neutron backscattering and spin-echo measurements of the diffuse scattering cross section. We find that the diffuse scattering intensity consists of emph{both} static and dynamic components. The static component first appears at the Curie temperature $Theta sim 400$ K, while the dynamic component freezes completely at the temperature T$_{f} sim 200$ K; together, these components account for all of the observed spectral weight contributing to the diffuse scattering cross section. The integrated intensity of the dynamic component peaks near the temperature at which the frequency-dependent dielectric constant reaches a maximum (T$_{max}$) when measured at 1 GHz, i. e. on a timescale of $sim 1$ ns. Our neutron scattering results can thus be directly related to dielectric and infra-red measurements of the polar nanoregions. Finally, the global temperature dependence of the diffuse scattering can be understood in terms of just two temperature scales, which is consistent with random field models.
High-temperature (T) and high-electric-field (E) effects on Pb[(Zn_{1/3} Nb_{2/3})_{0.92} Ti_{0.08}]O_3 (PZN-8%PT) were studied comprehensively by neutron diffraction in the ranges 300 <= T <= 550 K and 0 <= E <= 15 kV/cm. We have focused on how phase transitions depend on preceding thermal and electrical sequences. In the field cooling process (FC, E parallel [001] >= 0.5 kV/cm), a successive cubic (C) --> tetragonal (T) --> monoclinic (M_C) transition was observed. In the zero field cooling process (ZFC), however, we have found that the system does not transform to the rhombohedral (R) phase as widely believed, but to a new, unidentified phase, which we call X. X gives a Bragg peak profile similar to that expected for R, but the c-axis is always slightly shorter than the a-axis. As for field effects on the X phase, we found an irreversible X --> M_C transition via another monoclinic phase (M_A) as expected from a previous report [Noheda et al. Phys. Rev. Lett. 86, 3891 (2001)]. At a higher electric field, we confirmed a c-axis jump associated with the field-induced M_C --> T transition, which was observed by strain and x-ray diffraction measurements.
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