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We use neutron scattering and bulk property measurements to determine the single-ion crystal-field Hamiltonians of delafossites $rm KErSe_2$ and $rm CsErSe_2$. These two systems contains planar equilateral triangular Er lattices arranged in two stack ing variants: rhombohedral (for K) or hexagonal (Cs). Our analysis shows that regardless the stacking order both compound exhibit an easy-plane ground state doublet with large $J_z=1/2$ terms and the potential for significant quantum effects, making them candidates for quantum spin liquid or other exotic ground states.
139 - M. Matsuda , J. Ma , V. O. Garlea 2019
We report inelastic neutron scattering experiments in Ca2Y2Cu5O10 and map out the full one magnon dispersion which extends up to a record value of 53 meV for frustrated ferromagnetic (FM) edge-sharing CuO2 chain (FFESC) cuprates. A homogeneous spin-1 /2 chain model with a FM nearest-neighbor (NN), an antiferromagnetic (AFM) next-nearest-neighbor (NNN) inchain, and two diagonal AFM interchain couplings (ICs) analyzed within linear spin-wave theory (LSWT) reproduces well the observed strong dispersion along the chains and a weak one perpendicularly. The ratio R=|J_{a2}/J_{a1}| of the FM NN and the AFM NNN couplings is found as ~0.23, close to the critical point Rc=1/4 which separates ferromagnetically and antiferromagnetically correlated spiral magnetic ground states in single chains, whereas Rc>0.25 for coupled chains is considerably upshifted even for relatively weak IC. Although the measured dispersion can be described by homogeneous LSWT, the scattering intensity appears to be considerably reduced at ~11.5 and ~28 meV. The gap-like feature at 11.5 meV is attributed to magnon-phonon coupling whereas based on DMRG simulations of the dynamical structure factor the gap at 28 meV is considered to stem partly from quantum effects due to the AFM IC. Another contribution is ascribed to the intrinsic superstructure from the distorting incommensurate pattern of CaY cationic chains adjacent to the CuO2 ones. It gives rise to non-equivalent CuO4 units and Cu-O-Cu bond angles Phi and a resulting distribution of all exchange integrals. The Js fitted by homogeneous LSWT are regarded as average values. The record value of the FM NN integral J1=24 meV among FFESC cuprates can be explained by a non-universal Phi (not 90 deg.) and Cu-O bond length dependent anisotropic mean direct FM Cu-O exchange K_{pd}~120 meV. Enhanced K_{pd} values are also needed to compensate a significant AFM J_{dd} > ~6 meV.
La$_{1.67}$Sr$_{0.33}$NiO$_4$ develops charge and spin stripe orders at temperatures of roughly 200 K, with modulation wave vectors that are temperature independent. Various probes of spin and charge response have provided independent evidence for so me sort of change below $sim50$ K. In combination with a new set of neutron scattering measurements, we propose a unified interpretation of all of these observations in terms of a freezing of Ni-centered charges stripes, together with a glassy ordering of the spin stripes that shows up in neutron scattering as a slight rotation of the average spin direction.
Results of magnetization and neutron diffraction measurements of the manganese vanadate system Mn$_5$(VO$_4$)$_2$(OH)$_4$ are reported. The crystal structure of this compound contains triangular [Mn$_3$O$_{13}$] building blocks that produce two-dimen sional Mn$^{2+}$ magnetic networks with striped triangular topologies. The Mn sheets are connected through the nonmagnetic vanadate tetrahedra extending along the $a$-axis. Magnetization measurements performed on single crystals reveal the onset of a long-range antiferromagnetic order below approximately 45 K. The magnetic structure is N{e}el-type with nearest-neighbor Mn atoms coupled via three or four antiferromagnetic bonds. The magnetic moments are confined within the layers and are oriented parallel to the $b$ direction. The magnitudes of ordered moments are reduced, presumably by geometrical frustration and the low-dimensionality of the lattice structure.
The electronic ground state of Ca3LiOsO6 was recently considered within an intermediate coupling regime that revealed J=3/2 spin-orbit entangled magnetic moments. Through inelastic neutron scattering and density functional theory we investigate the m agnetic interactions and probe how the magnetism is influenced by the change in hierarchy of interactions as we move from Ca3LiOsO6 (5d3) to Ca3LiRuO6 (4d3). An alteration of the spin-gap and ordered local moment is observed, however the magnetic structure, Neel temperature and exchange interactions are unaltered. To explain this behavior it is necessary to include both spin-orbit coupling and hybridization, indicating the importance of an intermediate coupling approach when describing 5$d$ oxides.
The ferrimagnetic spinel $mathrm{CoV_2O_4}$ has been a topic of intense recent interest, both as a frustrated insulator with unquenched orbital degeneracy and as a near-itinerant magnet which can be driven metallic with moderate applied pressure. Her e, we report on our recent neutron diffraction and inelastic scattering measurements on powders with minimal cation site disorder. Our main new result is the identification of a weak ($frac{Delta a}{a} sim 10^{-4}$), first order structural phase transition at $T^*$ = 90 K, the same temperature where spin canting was seen in recent single crystal measurements. This transition is characterized by a short-range distortion of oxygen octahedral positions, and inelastic data further establish a weak $Deltasim 1.25 meV$ spin gap at low temperature. Together, these findings provide strong support for the local orbital picture and the existence of an orbital glass state at temperatures below $T^*$.
332 - J.-J. Wen , W. Tian , V. O. Garlea 2014
We describe why Ising spin chains with competing interactions in $rm SrHo_2O_4$ segregate into ordered and disordered ensembles at low temperatures ($T$). Using elastic neutron scattering, magnetization, and specific heat measurements, the two distin ct spin chains are inferred to have Neel ($uparrowdownarrowuparrowdownarrow$) and double-Neel ($uparrowuparrowdownarrowdownarrow$) ground states respectively. Below $T_mathrm{N}=0.68(2)$~K, the Neel chains develop three dimensional (3D) long range order (LRO), which arrests further thermal equilibration of the double-Neel chains so they remain in a disordered incommensurate state for $T$ below $T_mathrm{S}= 0.52(2)$~K. $rm SrHo_2O_4$ distills an important feature of incommensurate low dimensional magnetism: kinetically trapped topological defects in a quasi$-d-$dimensional spin system can preclude order in $d+1$ dimensions.
Results of magnetic field and temperature dependent neutron diffraction and magnetization measurements on oxy-arsenate Rb$_{2}$Fe$_{2}$O(AsO$_{4}$)$_{2}$ are reported. The crystal structure of this compound contains pseudo-one-dimensional [Fe$_{2}$O$ _{6}$]$^infty$ sawtooth-like chains, formed by corner sharing isosceles triangles of $Fe^{3+}$ ions occupying two nonequivalent crystallographic sites. The chains extend infinitely along the crystallographic $b$-axis and are structurally confined from one another via diamagnetic (AsO$_{4}$)$^{3-}$ units along the $a$-axis, and Rb$^+$ cations along the $c$-axis direction. Neutron diffraction measurements indicate the onset of a long range antiferromagnetic order below approximately 25 K. The magnetic structure consists of ferrimagnetic chains which are antiferromagnetically coupled with each other. Within each chain, one of the two Fe sites carries a moment which lies along the emph{b}-axis, while the second site bears a canted moment in the opposite direction. Externally applied magnetic field induces a transition to a ferrimagnetic state, in which the coupling between the sawtooth chains becomes ferromagnetic. Magnetization measurements performed on optically-aligned single crystals reveal evidence for an uncompensated magnetization at low magnetic fields that could emerge from to a phase-segregated state with ferrimagnetic inclusions or from antiferromagnetic domain walls. The observed magnetic states and the competition between them is expected to arise from strongly frustrated interactions within the sawtooth chains and relatively weak coupling between them.
103 - V. O. Garlea , R. Jin , E. Garlea 2012
We report the structural and magnetic properties of a new class of cobaltates with the chemical formula (BaSr)4-xLa2xCo4O15 (x = 0, 0.5 and 1). These compounds crystallize in a hexagonal structure in which cobalt ions are distributed among two distin ct crystallographic sites with different oxygen coordination. Three Co-O tetrahedra and one octahedron are linked by shared oxygen atoms to form Co4O15 clusters, which are packed together into a honeycomb-like network. Partial substitution of Sr and/or Ba atoms by La allows one to adjust the degree of Co valence mixing, but all compositions remain subject to a random distribution of charge. Magnetic susceptibility together with neutron scattering measurements reveal that all studied specimens are characterized by competing ferro- and antiferro-magnetic exchange interactions that give rise to a three dimensional Heisenberg spin-glass state. Neutron spectroscopy shows a clear trend of slowing down of spin-dynamics upon increasing La concentration, suggesting a reduction in charge randomness in the doped samples.
Magnetic order in the thermally quenched photomagnetic Prussian blue analogue coordination polymer K0.27Co[Fe(CN)6]0.73[D2O6]0.27 1.42D2O has been studied down to 4 K with unpolarized and polarized neutron powder diffraction as a function of applied magnetic field. Analysis of the data allows the onsite coherent magnetization of the Co and Fe spins to be established. Specifically, magnetic fields of 1 T and 4 T induce moments parallel to the applied field, and the sample behaves as a ferromagnet with a wandering axis.
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