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Magnetic interactions in disordered perovskite PbFe_{1/2}Nb_{1/2}O_3 and related compounds. Dominance of nearest-neighbor interaction

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 Added by Roman Kuzian
 Publication date 2013
  fields Physics
and research's language is English




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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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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.
135 - D. L. Huber 2008
The purpose of this note is to connect early work on thermal transport in spin-1/2 Heisenberg chains with uniaxial exchange anisotropy and nearest-neighbor interactions that was based on a moment analysis of the Fourier transform of the energy density correlation function with subsequent studies that make use of thermal current correlation functions.
Low-energy magnetic excitations in the spin-1/2 chain compound (C$_6$H$_9$N$_2$)CuCl$_3$ [known as (6MAP)CuCl$_3$] are probed by means of tunable-frequency electron spin resonance. Two modes with asymmetric (with respect to the $h u=gmu_B B$ line) frequency-field dependences are resolved, illuminating the striking incompatibility with a simple uniform $S=frac{1}{2}$ Heisenberg chain model. The unusual ESR spectrum is explained in terms of the recently developed theory for spin-1/2 chains, suggesting the important role of next-nearest-neighbor interactions in this compound. Our conclusion is supported by model calculations for the magnetic susceptibility of (6MAP)CuCl$_3$, revealing a good qualitative agreement with experiment.
The local atomic environments and magnetic properties were investigated for a series of Co(1+x)Fe(2-x)Si (0<x<1) Heusler compounds. While the total magnetic moment in these compounds increases with the number of valance electrons, the highest Curie temperature (Tc) in this series was found for Co1.5Fe1.5Si, with a Tc of 1069 K (24 K higher than the well known Co2FeSi). 57Fe Mossbauer spectroscopy was used to characterize the local atomic order and to estimate the Co and Fe magnetic moments. Consideration of the local magnetic moments and the exchange integrals is necessary to understand the trend in Tc.
We have investigated magnetic properties of Rb$_2$Cu$_2$Mo$_3$O$_{12}$ powder. Temperature dependence of magnetic susceptibility and magnetic-field dependence of magnetization have shown that this cuprate is a model compound of a one-dimensional spin-1/2 Heisenberg system with ferromagnetic first-nearest-neighbor (1NN) and antiferromagnetic second-nearest-neighbor (2NN) competing interactions (competing system). Values of the 1NN and 2NN interactions are estimated as $J_1 = -138$ K and $J_2 = 51$ K ($alpha equiv J_2 / J_1 = -0.37$). This value of $alpha$ suggests that the ground state is a spin-singlet incommensurate state. In spite of relatively large $J_1$ and $J_2$, no magnetic phase transition appears down to 2 K, while an antiferromagnetic transition occurs in other model compounds of the competing system with ferromagnetic 1NN interaction. For that reason, Rb$_2$Cu$_2$Mo$_3$O$_{12}$ is an ideal model compound to study properties of the incommensurate ground state that are unconfirmed experimentally.
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