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We have synthesized and studied single-crystal Ba5AlIr2O11 that featuresdimer chains of two inequivalent octahedra occupied by tetravalent andpentavalent ions, respectively. Ba5AlIr2O11 is a Mott insulator that undergoesa subtle structural phase transition near 210 K and a magnetic transition at4.5 K; the latter transition is surprisingly resistant to applied magneticfields up to 12 T, but sensitive to modest applied pressure. All resultsindicate that the phase transition at 210 K signals an enhanced charge orderthat induces electrical dipoles and strong dielectric response near 210 K. Itis clear that the strong covalency and spin-orbit interaction (SOI) suppressdouble exchange in Ir dimers and stabilize a novel magnetic state. The behaviorof Ba5AlIr2O11 therefore provides unique insights into the physics of SOI alongwith strong covalency in competition with double exchange interactions ofcomparable strength.

Coexisting charge and magnetic orders in the dimer-chain iridate Ba5AlIr2O11