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• W4300979694 abstract "The mixed-valent iridate ${mathrm{Ba}}_{3}{mathrm{InIr}}_{2}{mathrm{O}}_{9}$ has been discussed as a promising candidate for quantum spin-liquid behavior. The compound exhibits ${mathrm{Ir}}^{4.5+}$ ions in face-sharing ${mathrm{IrO}}_{6}$ octahedra forming ${mathrm{Ir}}_{2}{mathrm{O}}_{9}$ dimers with three ${t}_{2g}$ holes per dimer. Our results establish ${mathrm{Ba}}_{3}{mathrm{InIr}}_{2}{mathrm{O}}_{9}$ as a cluster Mott insulator. Strong intradimer hopping delocalizes the three ${t}_{2g}$ holes in quasimolecular dimer states while interdimer charge fluctuations are suppressed by Coulomb repulsion. The magnetism of ${mathrm{Ba}}_{3}{mathrm{InIr}}_{2}{mathrm{O}}_{9}$ emerges from spin-orbit entangled quasimolecular moments with yet unexplored interactions, opening up a new route to unconventional magnetic properties of $5d$ compounds. Using single-crystal x-ray diffraction we find the monoclinic space group $C2/c$ already at room temperature. Dielectric spectroscopy shows insulating behavior. Resonant inelastic x-ray scattering reveals a rich excitation spectrum below 1.5 eV with a sinusoidal dynamical structure factor that unambiguously demonstrates the quasimolecular character of the electronic states. Below 0.3 eV, we observe a series of excitations. According to exact diagonalization calculations, such low-energy excitations reflect the proximity of ${mathrm{Ba}}_{3}{mathrm{InIr}}_{2}{mathrm{O}}_{9}$ to a hopping-induced phase transition based on the condensation of a quasimolecular spin-orbit exciton. The dimer ground state roughly hosts two holes in a bonding $j=frac{1}{2}$ orbital and the third hole in a bonding $j=frac{3}{2}$ orbital." @default.
• W4300979694 created "2022-10-04" @default.
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• W4300979694 date "2022-10-04" @default.
• W4300979694 modified "2023-10-04" @default.
• W4300979694 title "Quasimolecular electronic structure of the spin-liquid candidate <mml:math xmlns:mml=http://www.w3.org/1998/Math/MathML><mml:msub><mml:mi mathvariant=normal>Ba</mml:mi><mml:mn>3</mml:mn></mml:msub><mml:msub><mml:mi mathvariant=normal>InIr</mml:mi><mml:mn>2</mml:mn></mml:msub><mml:msub><mml:mi mathvariant=normal>O</mml:mi><mml:mn>9</mml:mn></mml:msub></mml:math>" @default.
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