Subscribe to the gold package and get unlimited access to Shamra Academy
Register a new userDirect detection of dimer orbitals in Ba$_5$AlIr$_2$O$_{11}$
72
0
0.0
(
0
)
Ask ChatGPT about the research
No Arabic abstract
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.
rate research
Read More
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.
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$_{11}$.
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.
We have measured the specific heat of the coupled spin-dimer antiferromagnet Ba$_3$Mn$_2$O$_8$ to 50 mK in temperature and to 29 T in the magnetic field. The experiment extends to the midpoint of the field region (25.9 T $leq H leq$ 32.3 T) of the magnetization plateau at 1/2 of the saturation magnetization, and reveals the presence of three ordered phases in the field region between that of the magnetization plateau and the low-field spin-liquid region. The exponent of the phase boundary with the thermally disordered region is smaller than the theoretical value based on the Bose-Einstein condensation of spin triplets. At zero field and 29 T, the specific-heat data show gapped behaviors characteristic of spin liquids. The zero-field data indicate that the gapped triplet excitations form two levels whose energies differ by nearly a factor of two. At least the lower level is well localized. The data at 29 T reveal that the low-lying excitations at the magnetization plateau are weakly delocalized.
Non-reciprocal directional dichroism assigns an optical diode-like property to non-centrosymmetric magnets, making them appealing for low-dissipation optical devices. However, the direct electric control of this phenomenon at constant temperatures is scarce. In Ba$_2$CoGe$_2$O$_7$, we demonstrate the isothermal electric switch between domains possessing opposite magnetoelectric susceptibilities. Combining THz spectroscopy and multiboson spin-wave analysis, we show that unbalancing the domain population realizes the non-reciprocal light absorption of spin excitations.
Log in to be able to interact and post comments
comments
Fetching comments
Sign in to be able to follow your search criteria
