No Arabic abstract
We establish the double perovskite Ba$_2$CeIrO$_6$ as a nearly ideal model system for j=1/2 moments, with resonant inelastic x-ray scattering indicating a deviation of less than 1% from the ideally cubic j=1/2 state. The local j=1/2 moments form an fcc lattice and are found to order antiferromagnetically at $T_N$=14K, more than an order of magnitude below the Curie-Weiss temperature. Model calculations show that the geometric frustration of the fcc Heisenberg antiferromagnet is further enhanced by a next-nearest neighbor exchange, indicated by ab initio theory. Magnetic order is driven by a bond-directional Kitaev exchange and by local distortions via a strong magneto-elastic effect - both effects are typically not expected for j=1/2 compounds making Ba2CeIrO6 a riveting example for the rich physics of spin-orbit entangled Mott insulators.
Ba$_3$Mn$_2$O$_8$ is a geometrically frustrated spin dimer compound. We investigate the effect of site disorder on the zero field phase diagram of this material by considering the solid solution Ba$_{3}$(Mn$_{1-x}$V$_{x}$)$_{2}$O$_{8}$, where nonmagnetic V$^{5+}$ ions partially substitute magnetic Mn$^{5+}$ ions. This substitution results in unpaired $S=1$ moments for half-substituted dimers, which are ungapped and therefore susceptible to types of magnetic order not present in the parent compound. AC susceptibility measurements of compositions between $x=0.046$ and $x=0.84$ show a sharp frequency- and composition-dependent kink at temperatures below 210mK, suggesting that unpaired spins form a spin glass. The case for a glassy state is made clearer by the absence of any sharp features in the specific heat. However, Ba$_{3}$(Mn$_{1-x}$V$_{x}$)$_{2}$O$_{8}$ is not a paradigmatic spin glass. Whereas both the freezing temperature and the Weiss temperature (determined from susceptibility above 1K) vary strongly as a function of composition, the heat capacity per unpaired spin is found to be insensitive (above the glass transition) to the density of unpaired spins for the broad regime $0.18leq x leq 0.84$. This surprising result is consistent with a scenario in which nearest-neighbor unpaired spins form local, possibly fluctuating, spin-singlets prior to the eventual spin freezing. The spin glass state is only found for temperatures below the energy scale of single-ion anisotropy, suggestive this plays a significant role in determining the eventual ground state. Possible ground states in the dilute limit ($x < 0.04$ and $x > 0.9$) are also discussed.
$B$-site ordered 4$d^1$ and 5$d^1$ double perovskites have a number of potential novel ground states including multipolar order, quantum spin liquids and valence bond glass states. These arise from the complex interactions of spin-orbital entangled $J_{eff}$ = 3/2 pseudospins on the geometrically frustrated fcc lattice. The 4$d^1$ Mo$^{5+}$ perovskite Ba$_2$YMoO$_6$ has been suggested to have a valence bond glass ground state. Here we report on the low temperature properties of powder samples of isostructural Ba$_2$LuMoO$_6$: the only other known cubic 4$d^1$ perovskite with one magnetic cation. Our muon spectroscopy experiments show that magnetism in this material remains dynamic down to 60 mK without any spin freezing or magnetic order. A singlet-triplet excitation with a gap of $Delta$ = 28 meV is observed in inelastic neutron scattering. These results are interpreted as a disordered valence bond glass ground state similar to Ba$_2$YMoO$_6$. Our results highlight the differences of the 4$d^1$ double perovskites in comparison to cubic 5$d^1$ analogues, which have both magnetic and multipolar order.
The isostructural double perovskites Ba$_2$CuTeO$_6$ and Ba$_2$CuWO$_6$ are shown by theory and experiment to be frustrated square-lattice antiferromagnets with opposing dominant magnetic interactions. This is driven by differences in orbital hybridisation of Te$^{6+}$ and W$^{6+}$. A spin-liquid-like ground state is predicted for Ba$_2$Cu(Te$_{1-x}$W$_x$)O$_6$ solid solution similar to recent observations in Sr$_2$Cu(Te$_{1-x}$W$_x$)O$_6$.
We report the characterisation of natural samples of the cubic pyrite mineral MnS2 using very high resolution synchrotron X-ray diffraction techniques. At low temperatures we find a new low temperature polymorph, which results from coupling between magnetic and lattice degrees of freedom. Below the magnetic ordering temperature T_N= 48 K, we detect a pseudo-tetragonal distortion with a tiny c/a ratio of 1.0006. The structure can be refined in the space group Pbca. The symmetry lowering reduces magnetic frustration in the fcc Mn2+ lattice and is likely responsible for the previously reported lock-in of the magnetic propagation vector. This behaviour is similar to the frustration driven symmetry breaking reported in other three-dimensional Heisenberg magnets like the chromate spinels
The search for flat-band solid-state realizations is a crucial issue to verify or to challenge theoretical predictions for quantum many-body flat-band systems. For frustrated quantum magnets flat bands lead to various unconventional properties related to the existence of localized many-magnon states. The recently synthesized magnetic compound Ba$_2$CoSi$_2$O$_6$Cl$_2$ seems to be an almost perfect candidate to observe these features in experiments. We develop a theory for Ba$_2$CoSi$_2$O$_6$Cl$_2$ by adapting the localized-magnon concept to this compound. We first show that our theory describes the known experimental facts and then we propose new experimental studies to detect a field-driven phase transition related to a Wigner-crystal-like ordering of localized magnons at low temperatures.