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We synthesize and study single crystals of the layered honeycomb lattice Mottinsulators Na2RuO3 and Li2RuO3 with magnetic Ru4+(4d4) ions. The newly foundNa2RuO3 features a nearly ideal honeycomb lattice and ordersantiferromagnetically at 30 K. Single-crystals of Li2RuO3 adopt a honeycomblattice with either C2/m or more distorted P21/m below 300 K, depending ondetailed synthesis conditions. We find that Li2RuO3 in both structures hosts awell-defined magnetic state, in contrast to the singlet ground state found inpolycrystalline Li2RuO3. A phase diagram generated based on our resultsuncovers a new, direct correlation between the magnetic ground state andbasal-plane distortions in the honeycomb ruthenates.

Lattice-Tuned Magnetism of Ru4+(4d4) Ions in Single-Crystals of the Layered Honeycomb Ruthenates: Li2RuO3 and Na2RuO3