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Register a new userCharge ordering in Ir dimers in the ground state of Ba$_5$AlIr$_2$O$_{11}$
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Added by
Vamshi Mohan Katukuri
Publication date
2021
fields
Physics
and research's language is
English
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It has been well established experimentally that the interplay of electronic correlations and spin-orbit interactions in Ir$^{4+}$ and Ir$^{5+}$ oxides results in insulating J$_{rm eff}$=1/2 and J$_{rm eff}$=0 ground states, respectively. However, in compounds where the structural dimerization of iridum ions is favourable, the direct Ir $d$--$d$ hybridisation can be significant and takes a key role. Here, we investigate the effects of direct Ir $d$--$d$ hybridisation in comparison with electronic correlations and spin-orbit coupling in Ba$_5$AlIr$_2$O$_{11}$, a compound with Ir dimers. Using a combination of $ab$ $initio$ many-body wave function quantum chemistry calculations and resonant inelastic X-ray scattering (RIXS) experiments, we elucidate the electronic structure of Ba$_5$AlIr$_2$O$_{11}$. We find excellent agreement between the calculated and the measured spin-orbit excitations. Contrary to the expectations, the analysis of the many-body wave function shows that the two Ir (Ir$^{4+}$ and Ir$^{5+}$) ions in the Ir$_2$O$_9$ dimer unit in this compound preserve their local J$_{rm eff}$ character close to 1/2 and 0, respectively. The local point group symmetry at each of the Ir sites assumes an important role, significantly limiting the direct $d$--$d$ hybridisation. Our results emphasize that minute details in the local crystal field (CF) environment can lead to dramatic differences in electronic states in iridates and 5$d$ oxides in general.
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The electronic states of many Mott insulators, including iridates, are often conceptualized in terms of localized atomic states such as the famous $J_text{eff}=1/2$ state. Although, orbital hybridization can strongly modify such states and dramatically change the electronic properties of materials, probing this process is highly challenging. In this work, we directly detect and quantify the formation of dimer orbitals in an iridate material Ba$_5$AlIr$_2$O$_{11}$ using resonant inelastic x-ray scattering (RIXS). Sharp peaks corresponding to the excitations of dimer orbitals are observed and analyzed by a combination of density functional theory (DFT) calculations and theoretical simulations based on a Ir-Ir cluster model. Such partially delocalized dimer states lead to a re-definition of the angular momentum of the electrons and changes in the magnetic and electronic behaviors of the material. We use this to explain the reduction of the observed magnetic moment with respect to prediction based on atomic states. This study opens new directions to study dimerization in a large family of materials including solids, heterostructures, molecules and transient states.
We study low energy excitations in the quantum breathing pyrochlore antiferromagnet Ba$_3$Yb$_2$Zn$_5$O$_{11}$ by combination of inelastic neutron scattering (INS) and thermodynamical properties measurements. The INS spectra are quantitatively explained by spin-1/2 single-tetrahedron model having $XXZ$ anisotropy and Dzyaloshinskii-Moriya interaction. This model has a two-fold degeneracy of the lowest-energy state per tetrahedron and well reproduces the magnetization curve at 0.5 K and heat capacity above 1.5 K. At lower temperatures, however, we observe a broad maximum in the heat capacity around 63 mK, demonstrating that a unique quantum ground state is selected due to extra perturbations with energy scale smaller than the instrumental resolution of INS.
The breathing pyrochlore lattice material Ba$_3$Yb$_2$Zn$_5$O$_{11}$ exists in the nearly decoupled limit, in contrast to most other well-studied breathing pyrochlore compounds. As a result, it constitutes a useful platform to benchmark theoretical calculations of exchange interactions in insulating Yb$^{3+}$ magnets. Here we study Ba$_3$Yb$_2$Zn$_5$O$_{11}$ at low temperatures in applied magnetic fields as a further probe of the physics of this model system. Experimentally, we consider the behavior of polycrystalline samples of Ba$_3$Yb$_2$Zn$_5$O$_{11}$ with a combination of inelastic neutron scattering and heat capacity measurements down to 75 mK and up to fields of 10 T. Consistent with previous work, inelastic neutron scattering finds a level crossing near 3 T, but no significant dispersion of the spin excitations is detected up to the highest applied fields. Refinement of the theoretical model previously determined at zero field can reproduce much of the inelastic neutron scattering spectra and specific heat data. A notable exception is a low temperature peak in the specific heat near 0.1 K. This may indicate the scale of interactions between tetrahedra or may reflect undetected disorder in Ba$_3$Yb$_2$Zn$_5$O$_{11}$.
Magnetic susceptibility and the magnetization process have been measured in green polycrystal. In this compound, the magnetic manganese ion exists as Mn$^{5+}$ in a tetrahedral environment, and thus the magnetic interaction can be described by an S=1 Heisenberg model. The ground state was found to be a spin singlet with an excitation gap $Delta/k_{rm B}=11.2$ K. Magnetization plateaus were observed at zero and at half of the saturation magnetization. These results indicate that the present system can be represented by a coupled antiferromagnetic dimer model.
We study the thermodynamic and high-magnetic-field properties of the magnetic insulator Ba$_5$CuIr$_3$O$_{12}$, which shows no magnetic order down to 2 K consistent with a spin liquid ground state. While the temperature dependence of the magnetic susceptibility and the specific heat shows only weak antiferromagnetic correlations, we find that the magnetization does not saturate up to a field of 59 Tesla, leading to an apparent contradiction. We demonstrate that the paradox can be resolved, and all of the experimental data can be consistently described within the framework of random singlet states. We demonstrate a generic procedure to derive the exchange coupling distribution $P(J)$ from the magnetization measurements and use it to show that the experimental data is consistent with the power-law form $P(J)sim J^{-alpha}$ with $alpha approx 0.6 $. Thus, we reveal that high-magnetic-field measurements can be essential to discern quantum spin liquid candidates from disorder dominated states that do not exhibit long-range order.
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