Lattice-tuned magnetism of Ru4+(4d4) ions in single crystals of the layered honeycomb ruthenates Li2RuO3 and Na2RuO3

We synthesize and study single crystals of the layered honeycomb lattice Mott insulators Na2RuO3 and Li2RuO3 with magnetic Ru4+(4d(4)) ions. The newly found Na2RuO3 features a nearly ideal honeycomb lattice and orders antiferromagnetically at 30 K. Single crystals of Li2RuO3 adopt a honeycomb lattice with either C2/m or more distorted P2(1)/m below 300 K, depending on detailed synthesis conditions. We find that Li2RuO3 in both structures hosts a well-defined magnetic state, in contrast to the singlet ground state found in polycrystalline Li2RuO3. A phase diagram generated based on our results uncovers a new, direct correlation between the magnetic ground state and basal-plane distortions in the honeycomb ruthenates.