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We show that the valence electrons of Ba3NaRu2O9, which has a quasi-molecularstructure, completely crystallize below 210 K. Using an extended Hubbard model,we show that the charge ordering instability results from long-range Coulombinteractions. However, orbital ordering, metal-metal bonding and formation of apartial spin gap enforce the magnitude of the charge separation. The stripedcharge order and frustrated hcp lattice of Ru2O9 dimers lead to competitionwith a quasi-degenerate charge-melted phase under photo-excitation at lowtemperature. Our results establish a broad class of simple metal oxides asmodels for emergent phenomena at the border between the molecular and solidstates.

Charge order at the frontier between the molecular and solid states in Ba3NaRu2O9