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Neutron diffraction, magnetization, resistivity, and heat capacitymeasurements on the 6H-perovskite Ba3BiRu2O9 reveal simultaneous magnetic andstructural dimerization driven by strong magnetoelastic coupling. Anisostructural but strongly displacive first-order transition on cooling throughT*=176 K is associated with a change in the nature of direct Ru-Ru bonds withinRu2O9 face-sharing octahedra. Above T*, Ba3BiRu2O9 is an S=1 magnetic dimersystem with intradimer exchange interactions J0/kB=320 K and interdimerexchange interactions J'/kB=-160 K. Below T*, a spin-gapped state emerges with\Delta\approx220 K. Ab initio calculations confirm antiferromagnetic exchangewithin dimers, but the transition is not accompanied by long range-magneticorder.

Spin-gap opening accompanied by a strong magnetoelastic response in the S=1 magnetic dimer system Ba3BiRu2O9