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Manifolds of magnetic ordered states and excitations in the almost Heisenberg pyrochlore antiferromagnet MgCr2O4

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 Added by Oksana Zaharko
 Publication date 2018
  fields Physics
and research's language is English




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In spinels ACr2O4 (A=Mg, Zn) realisation of the classical pyrochlore Heisenberg antiferromagnet model is complicated by a strong spin-lattice coupling: the extensive degeneracy of the ground state is lifted by a magneto-structural transition at TN=12.5 K. We study the resulting low-temperature low-symmetry crystal structure by synchrotron x-ray diffraction. The consistent features of x-ray low-temperature patterns are explained by the tetragonal model of Ehrenberg et. al (Pow. Diff. 17, 230( 2002)), while other features depend on sample or cooling protocol. Complex partially ordered magnetic state is studied by neutron diffraction and spherical neutron polarimetry. Multiple magnetic domains of configuration arms of the propagation vectors k1=(1/2 1/2 0), k2=(1 0 1/2) appear. The ordered moment reaches 1.94(3) muB/Cr3+ for k1 and 2.08(3) muB/Cr3+ for k2, if equal amount of the k1 and k2 phases is assumed. The magnetic arrangements have the dominant components along the [110] and [1-10] diagonals and a smaller c-component. By inelastic neutron scattering we investigate the spin excitations, which comprise a mixture of dispersive spin waves propagating from the magnetic Bragg peaks and resonance modes centered at equal energy steps of 4.5 meV. We interpret these as acoustic and optical spin wave branches, but show that the neutron scattering cross sections of transitions within a unit of two corner-sharing tetrahedra match the observed intensity distribution of the resonances. The distinctive fingerprint of cluster-like excitations in the optical spin wave branches suggests that propagating excitations are localized by the complex crystal structure and magnetic orders.



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We report a comprehensive inelastic neutron-scattering study of the frustrated pyrochlore antiferromagnet MgCr2O4 in its cooperative paramagnetic regime. Theoretical modeling yields a microscopic Heisenberg model with exchange interactions up to third-nearest neighbors, which quantitatively explains all the details of the dynamic magnetic response. Our work demonstrates that the magnetic excitations in paramagnetic MgCr2O4 are faithfully represented in the entire Brillouin zone by a theory of magnons propagating in a highly-correlated paramagnetic background. Our results also suggest that MgCr2O4 is proximate to a spiral spin-liquid phase distinct from the Coulomb phase, which has implications for the magneto-structural phase transition in MgCr2O4 .
We use the rotation-invariant Greens function method (RGM) and the high-temperature expansion (HTE) to study the thermodynamic properties of the Heisenberg antiferromagnet on the pyrochlore lattice. We discuss the excitation spectra as well as various thermodynamic quantities, such as spin correlations, uniform susceptibility, specific heat and static and dynamical structure factors. For the ground state we present RGM data for arbitrary spin quantum numbers $S$. At finite temperatures we focus on the extreme quantum cases $S=1/2$ and $S=1$. We do not find indications for magnetic long-range order for any value of $S$. We discuss the width of the pinch point in the static structure factor in dependence on temperature and spin quantum number. We compare our data with experimental results for the pyrochlore compound NaCaNi$_2$F$_7$ ($S=1$). Thus, our results for the dynamical structure factor agree well with the experimentally observed features at 3 ldots 8~meV for NaCaNi$_2$F$_7$. We analyze the static structure factor ${S}_{bf q}$ to find regions of maximal ${S}_{bf q}$. The high-temperature series of the ${S}_{bf q}$ provide a fingerprint of weak {it order by disorder} selection of a collinear spin structure, where (classically) the total spin vanishes on each tetrahedron and neighboring tetrahedra are dephased by $pi$.
The XY-pyrochlore antiferromagnet ETO is studied by heat capacity measurements and electron spin resonance spectroscopy performed on single crystal samples. The magnetic phase diagrams are established for two directions of applied field, $Hparallel [100]$ and $Hparallel [111]$. In the magnetically ordered phase observed below $T_N=1.2$ K, the magnetic excitation spectrum consists of a Goldstone mode acquiring an isotropic gap in an applied field, and another mode with a gap softening in the vicinity of a field-induced phase transition. This second-order transition takes place at a critical field $H_c$ above which the magnetization process is accompanied by a canting of the magnetic moments off their local easy-planes. The specific heat curves for $Hparallel [100]$ ($Hgg H_c$) are well described by a model presuming a single dispersionless excitation mode with the energy gap obtained from the spectroscopic measurements.
264 - J. Xu , V. K. Anand , A. K. Bera 2015
We present synchrotron x-ray diffraction, neutron powder diffraction and time-of-flight inelastic neutron scattering measurements on the rare earth pyrochlore oxide Nd2Zr2O7 to study the ordered state magnetic structure and cystal field states. The structural characterization by high-resolution synchrotron x-ray diffraction confirms that the pyrochlore structure has no detectable O vacancies or Nd/Zr site mixing. The neutron diffraction reveals long range all-in/all-out antiferromagnetic order below T_N ~ 0.4 K with propagation vector k = (0 0 0) and an ordered moment of 1.26(2) mu_B/Nd at 0.1 K. The ordered moment is much smaller than the estimated moment of 2.65 mu_B/Nd for the local <111> Ising ground state of Nd3+ (J=9/2) suggesting that the ordering is partially suppressed by quantum fluctuations. The strong Ising anisotropy is further confirmed by the inelastic neutron scattering data which reveals a well-isolated dipolar-octupolar type Kramers doublet ground state. The crystal field level scheme and ground state wavefunction have been determined.
The gadolinium pyrochlores, Gd$_2B_2$O$_7$, are amongst the best realizations of antiferromagnetically coupled Heisenberg spins on a pyrochlore lattice. We present a magnetic characterization of Gd$_2$Pt$_2$O$_7$, a unique member of this family. Magnetic susceptibility, heat capacity, and muon spin relaxation measurements show that Gd$_2$Pt$_2$O$_7$ undergoes an antiferromagnetic ordering transition at $T_N = 1.6$ K. This transition is strongly first order, as indicated by the sharpness of the heat capacity anomaly, thermal hysteresis in the magnetic susceptibility, and a non-divergent relaxation rate in $mu$SR. The form of the heat capacity below $T_N$ suggests that the ground state is an anisotropic collinear antiferromagnet with an excitation spectrum that is gapped by 0.245(1) meV. The ordering temperature in Gd$_2$Pt$_2$O$_7$, $T_N = 1.6$ K, is a substantial 160% increase from other gadolinium pyrochlores, which have been found to order at 1 K or lower. We attribute this enhancement in $T_N$ to the $B$-site cation, platinum, which, despite being non-magnetic, has a filled $5d$ $t_{2g}$ orbital and an empty $5d$ $e_g$ orbital that can facilitate superexchange. Thus, the magnetic frustration in Gd$_2$Pt$_2$O$_7$ is partially relieved, thereby promoting magnetic order.
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