No Arabic abstract
We report the structural transformation of hexagonal Ba3YIr2O9 to a cubic double perovskite form (stable in ambient conditions) under an applied pressure of 8GPa at 1273K. While the ambient pressure (AP) synthesized sample undergoes long-range magnetic ordering at 4K, the high pressure(HP) synthesized sample does not order down to 2K as evidenced from our susceptibility, heat capacity and nuclear magnetic resonance (NMR) measurements. Further, for the HP sample, our heat capacity data have the form gamma*T+beta*T3 in the temperature (T) range of 2-10K with the Sommerfeld coefficient gamma=10mJ/mol-Ir K2. The 89Y NMR shift has no T-dependence in the range of 4-120K and its spin-lattice relaxation rate varies linearly with T in the range of 8-45K (above which it is T-independent). Resistance measurements of both the samples confirm that they are semiconducting. Our data provide evidence for the formation of a 5d based, gapless, quantum spin-liquid (QSL) in the cubic (HP) phase of Ba3YIr2O9. In this picture, the T term in the heat capacity and the linear variation of 89Y 1/T1 arises from excitations out of a spinon Fermi surface. Our findings lend credence to the theoretical suggestion [G. Chen, R. Pereira, and L. Balents, Phys. Rev. B 82, 174440 (2010)] that strong spin-orbit coupling can enhance quantum fluctuations and lead to a QSL state in the double perovskite lattice.
The magnetic structure of Ca$_2$MnReO$_6$ double perovskite is investigated by neutron powder diffraction and bulk magnetization, showing dominant non-collinear Mn magnetic moments [$4.35(7)$ $mu_B$] that are orthogonally aligned with the small Re moments [$0.22(4)$ $mu_B$]. $Ab$-initio electronic structure calculations show that the strong spin-orbit coupling for Re $5d$ electrons combined with a relatively modest on-site Coulomb repulsion ($U_{eff}^{Re} gtrsim 0.6$ eV) is sufficient to render this material insulating. This is a rare example of spin-orbit assisted Mott insulator outside the realm of iridates, with remarkable magnetic properties.
We show that the off-diagonal exchange anisotropy drives Mott insulators with strong spin-orbit coupling to a classical spin liquid regime, characterized by an infinite number of ground states and Ising variables living on closed or open strings. Depending on the sign of the anisotropy, quantum fluctuations either fail to lift the degeneracy down to very low temperatures, or select non-collinear magnetic states with unconventional spin correlations. The results apply to all 2D and 3D tri-coordinated materials with bond-directional anisotropy, and provide a consistent interpretation of the suppression of the x-ray magnetic circular dichroism signal reported recently for $beta$-Li$_2$IrO$_3$ under pressure.
We report muSR experiments on Mg{x}Cu{4-x}(OH)6Cl2 with x sim 1, a new material isostructural to Herbertsmithite exhibiting regular kagome planes of spin 1/2 (Cu^{2+}), and therefore a candidate for a spin liquid ground state. We evidence the absence of any magnetic ordering down to 20 mK (sim J/10^4). We investigate in detail the spin dynamics on well characterized samples in zero and applied longitudinal fields and propose a low T defect based interpretation to explain the unconventional dynamics observed in the quantum spin liquid phase.
We report neutron scattering experiments which reveal a large spin gap in the magnetic excitation spectrum of weakly-monoclinic double perovskite Sr2ScOsO6. The spin gap is demonstrative of appreciable spin-orbit-induced anisotropy, despite nominally orbitally-quenched 5d3 Os5+ ions. The system is successfully modeled including nearest neighbor interactions in a Heisenberg Hamiltonian with exchange anisotropy. We find that the presence of the spin-orbit-induced anisotropy is essential for the realization of the type I antiferromagnetic ground state. This demonstrates that physics beyond the LS or JJ coupling limits plays an active role in determining the collective properties of 4d3 and 5d3 systems, and that theoretical treatments must include spin-orbit coupling.
CuAl2O4 is a normal spinel oxide having quantum spin, S=1/2 for Cu2+. It is a rather unique feature that the Cu2+ ions of CuAl2O4 sit at a tetrahedral position, not like the usual octahedral position for many oxides. At low temperatures, it exhibits all the thermodynamic evidence of a quantum spin glass. For example, the polycrystalline CuAl2O4 shows a cusp centered at ~2 K in the low-field dc magnetization data and a clear frequency dependence in the ac magnetic susceptibility while it displays logarithmic relaxation behavior in a time dependence of the magnetization. At the same time, there is a peak at ~2.3 K in the heat capacity, which shifts towards higher temperature with magnetic fields. On the other hand, there is no evidence of new superlattice peaks in the high-resolution neutron powder diffraction data when cooled from 40 to 0.4 K. This implies that there is no long-ranged magnetic order down to 0.4 K, thus confirming a spin glass-like ground state for CuAl2O4. Interestingly, there is no sign of structural distortion either although Cu2+ is a Jahn-Teller active ion. Thus, we claim that an orbital liquid state is the most likely ground state in CuAl2O4. Of further interest, it also exhibits a large frustration parameter, f = Theta_CW/Tm ~67, one of the largest values reported for spinel oxides. Our observations suggest that CuAl2O4 should be a rare example of a frustrated quantum spin glass with a good candidate for an orbital liquid state.