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We report structural, magnetic, transport and thermal properties ofsingle-crystal Ca2Ru1-xIrxO4 (0 < x< 0.65). Ca2RuO4 is a structurally-drivenMott insulator with a metal-insulator transition at TMI = 357 K, which is wellseparated from antiferromagnetic order at TN = 110 K. Substitution of 5delement, Ir, for Ru enhances spin-orbit coupling (SOC) and locking between thestructural distortions and magnetic moment canting. In particular, Ir dopingintensifies the distortion or rotation of Ru/IrO6 octahedra and induces weakferromagnetic behavior along the c-axis. Moreover, the magnetic orderingtemperature TN increases from 110 K at x = 0 to 215 K with enhanced magneticanisotropy at x = 0.65. The effect of Ir doping sharply contrasts with that of3d-element doping such as Cr, Mn and Fe, which suppresses TN and inducesunusual negative volume thermal expansion. The stark difference between 3d- and5d-element doping underlines a strong magnetoelastic coupling inherent in theIr-rich oxides.

Evolution of Magnetism in Single-Crystal Ca2Ru1-xIrxO4 (0< x <0.65)