Spin-gap opening accompanied by a strong magnetoelastic response in the S=1 magnetic dimer system Ba3BiRu2O9

Neutron diffraction, magnetization, resistivity, and heat capacity measurements on the 6H-perovskite Ba3BiRu2O9 reveal simultaneous magnetic and structural dimerization driven by strong magnetoelastic coupling. An isostructural but strongly displacive first-order transition on cooling through T*=176 K is associated with a change in the nature of direct Ru-Ru bonds within Ru2O9 face-sharing octahedra. Above T*, Ba3BiRu2O9 is an S=1 magnetic dimer system with intradimer exchange interactions J0/kB=320 K and interdimer exchange interactions J'/kB=-160 K. Below T*, a spin-gapped state emerges with \Delta\approx220 K. Ab initio calculations confirm antiferromagnetic exchange within dimers, but the transition is not accompanied by long range-magnetic order.Comment: 5 pages, 5 figures, accepted by Physical Review

Magnetic anomalies in the spin chain system, Sr3_3Cu1−x_{1-x}Znx_xIrO6_6

We report the results of ac and dc magnetization (M) and heat-capacity (C) measurements on the solid solution, Sr$_3$Cu$_{1-x}$Zn$_x$IrO$_6$. While the Zn end member is known to form in a rhombohedral pseudo one-dimensional K$_4$CdCl$_6$ structure with an antiferromagnetic ordering temperature of (T$_N$ =) 19 K, the Cu end member has been reported to form in a monoclinically distorted form with a Curie temperature of (T$_C$ =) 19 K. The magnetism of the Zn compound is found to be robust to synthetic conditions and is broadly consistent with the behavior known in the literature. However, we find a lower magnetic ordering temperature (T$_o$) for our Cu compound (~ 13 K), thereby suggesting that T$_o$ is sensitive to synthetic conditions. The Cu sample appears to be in a spin-glass-like state at low temperatures, judged by a frequency dependence of ac magnetic susceptibility and a broadening of the C anomaly at the onset of magnetic ordering, in sharp contrast to earlier proposals. Small applications of magnetic field, however, drive this system to ferromagnetism as inferred from the M data. Small substitutions for Cu/Zn (x = 0.75 or 0.25) significantly depress magnetic ordering; in other words, T$_o$ varies non-monotonically with x (T$_o$ ~ 6, 3 and 4 K for x = 0.25, 0.5, and 0.67 respectively). The plot of inverse susceptibility versus temperature is non-linear in the paramagnetic state as if correlations within (or among) the magnetic chains continuously vary with temperature. The results establishComment: 7 pages, 7 figures, Revte

Random interactions and spin-glass thermodynamic transition in the hole-doped Haldane system Y2−x_{2-x}Cax_xBaNiO5_5

Magnetization, DC and AC bulk susceptibility of the $S$=1 Haldane chain system doped with electronic holes, Y$_{2-x}$Ca$_x$BaNiO$_5$ (0$\leq$x$\leq$0.20), have been measured and analyzed. The most striking results are (i) a sub-Curie power law behavior of the linear susceptibility, $\chi (T)$$\sim$ $T$$^{-\alpha}$, for temperature lower than the Haldane gap of the undoped compound (x=0) (ii) the existence of a spin-glass thermodynamic transition at $T$$_g$ = 2-3 K. These findings are consistent with (i) random couplings within the chains between the spin degrees of freedom induced by hole doping, (ii) the existence of ferromagnetic bonds that induce magnetic frustration when interchain interactions come into play at low temperature.Comment: 4 pages, 4 figures, to appear in Phys. Rev.

Coexistence of Haldane gap excitations and long range antiferromagnetic order in mixed-spin nickelates R_2 Ba Ni O_5

The spin dynamics of the S=1 Ni-chains in mixed-spin antiferromagnets Pr_2 Ba Ni O_5 and Nd_x Y_2-x Ba Ni O_5 is described in terms of a simple Ginzburg-Landau Lagrangian coupled to the sublattice of rare-earth ions. Within this framework we obtain a theoretical explanation for the experimentally observed coexistence of Haldane gap excitations and long-range magnetic order, as well as for the increase of the Haldane gap energy below the Neel point. We also predict that the degeneracy of the Haldane triplet is lifted in the magnetically ordered phase. The theoretical results are consistent with the available experimental data.Comment: 4 pages, 1 figure, submitted to PRL An alternative derivation of main results and new references adde

Anomalous spectral weight in photoemission spectra of the hole doped Haldane chain Y2-xSrxBaNiO5

In this paper, we present photoemission experiments on the hole doped Haldane chain compound $Y_{2-x}Sr_xBaNiO_5$. By using the photon energy dependence of the photoemission cross section, we identified the symmetry of the first ionisation states (d type). Hole doping in this system leads to a significant increase in the spectral weight at the top of the valence band without any change in the vicinity of the Fermi energy. This behavior, not observed in other charge transfer oxides at low doping level, could result from the inhomogeneous character of the doped system and from a Ni 3d-O 2p hybridization enhancement due to the shortening of the relevant Ni-O distance in the localized hole-doped regions.Comment: 5 pages, 4 figure

An experimental measurement of the staggered magnetization curve for a Haldane spin chain

Long-range magnetic ordering in R_2 Ba Ni O_5 (R=magnetic rare earth) quasi-1-dimensional mixed-spin antiferromagnets is described by a simple mean-field model that is based on the intrinsic staggered magnetization function of isolated Haldane spin chains for the Ni-subsystem, and single-ion magnetization functions for the rare earth ions. The model is applied to new experimental results obtained in powder diffraction experiments on Nd_2 Ba Ni O_5 and Nd Y Ba Ni O_5, and to previously published diffraction data for Er_2 Ba Ni O_5. From this analysis we extract the bare staggered magnetization curve for Haldane spin chains in these compounds.Comment: some revisions in text and figures 5 pages, 2 figures, PRL accepted for publicatio

Magnetic ordering, spin waves, and Haldane gap excitations in (Nd_x Y_{1-x})_2 Ba Ni O_5 linear-chain mixed-spin antiferromagnets

Linear-chain nickelates with the composition (Nd_x Y_{1-x})_2 Ba Ni O_5 (x=1, x=0.75, x=0.5, and x=0.25) are studied in a series of neutron scattering experiments. Powder diffraction is used to determine the temperature dependence of the magnetic structure in all four systems. Single-crystal inelastic neutron scattering is employed to investigate the temperature dependence of the Haldane-gap excitations and low-energy spin waves in the x=1 compound Nd_2 Ba Ni O_5. The results of these experiments are discussed in the context of the ``Haldane chain in a staggered field'' model for R_2 Ba Ni O_5 systems, and quantitative agreement with theory is obtained.Comment: Major rewriting and inclusion of new experimental data 30 pages, 14 figure

Spin-Wave Description of Haldane-gap antiferromagnets

Modifying the conventional antiferromagnetic spin-wave theory which is plagued by the difficulty of the zero-field sublattice magnetizations diverging in one dimension, we describe magnetic properties of Haldane-gap antiferromagnets. The modified spin waves, constituting a grand canonical bosonic ensemble so as to recover the sublattice symmetry, not only depict well the ground-state correlations but also give useful information on the finite-temperature properties.Comment: to be published in J. Phys. Soc. Jpn. Vol. 72, No. 4 (2003

Impurities in s=1s=1 Heisenberg Antiferromagnets

The $s=1$ Heisenberg Antiferromagnet is studied in the presence of two kinds of local impurities. First, a perturbed antiferromagnetic bond with $J'\ne J$ at the center of an even-length open chain is considered. Using the density matrix renormalization group method we find that, for sufficiently strong or weak $J'$, a bound state is localized at the impurity site, giving rise to an energy level in the Haldane gap. The energy of the bound state is in agreement with perturbative results, based on $s=1/2$ chain-end excitations, both in the weak and strong coupling limit. In a region around the uniform limit, $J'=J$, no states are found with energy below the Haldane gap. Secondly, a $s=1/2$ impurity at the center of an otherwise even-length open chain is considered. The coupling to the $s=1/2$ impurity is varied. Bound states in the Haldane gap are found {\it only} for sufficiently weak (antiferromagnetic) coupling. For a $s=1/2$ impurity coupled with a strong (antiferromagnetic) bond, {\it no} states are found in the Haldane. Our results are in good qualitative agreement with recent experiments on doped NENP and Y$_2$BaNiO$_5$.Comment: 29 pages, RevTeX 3.0, 12 uuencoded postscript figures include