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The mixed-valent iridate Ba3InIr2O9 has been discussed as a promisingcandidate for quantum spin-liquid behavior. The compound exhibits Ir$^{4.5+}$ions in face-sharing IrO6 octahedra forming Ir2O9 dimers with three t2g holesper dimer. Our results establish Ba3InIr2O9 as a cluster Mott insulator. Strongintra-dimer hopping delocalizes the three t2g holes in quasi-molecular dimerstates while inter-dimer charge fluctuations are suppressed by Coulombrepulsion. The magnetism of Ba3InIr2O9 emerges from spin-orbit entangledquasi-molecular moments with yet unexplored interactions, opening up a newroute to unconventional magnetic properties of 5d compounds. Usingsingle-crystal x-ray diffraction we find the monoclinic space group C2/calready at room temperature. Dielectric spectroscopy shows insulating behavior.Resonant inelastic x-ray scattering (RIXS) reveals a rich excitation spectrumbelow 1.5 eV with a sinusoidal dynamical structure factor that unambiguouslydemonstrates the quasi-molecular character of the electronic states. Below 0.3eV, we observe a series of excitations. According to exact diagonalizationcalculations, such low-energy excitations reflect the proximity of Ba3InIr2O9to a hopping-induced phase transition based on the condensation of aquasi-molecular spin-orbit exciton. The dimer ground state roughly hosts twoholes in a bonding j=1/2 orbital and the third hole in a bonding j=3/2 orbital.

Quasimolecular electronic structure of the spin-liquid candidate Ba$_3$InIr$_2$O$_9$