We report structural, magnetic, transport, and thermal properties of single-crystal Ca2Ru1−xIrxO4(0≤x≤0.65). Ca2RuO4 is a structurally driven Mott insulator with a metal-insulator transition at TMI=357K, which is well separated from antiferromagnetic order at TN=110K. Substitution of a 5d element, Ir, for Ru enhances spin-orbit coupling and locking between the structural distortions and magnetic moment canting. Ir doping intensifies the distortion or rotation of Ru/IrO6 octahedra and induces weak ferromagnetic behavior along the c axis. In particular, Ir doping suppresses TN but concurrently causes an additional magnetic ordering TN2 at a higher temperature up to 210 K for x=0.65. The effect of Ir doping sharply contrasts with that of 3d-element doping such as Cr, Mn, and Fe, which suppresses TN and induces unusual negative volume thermal expansion. The stark difference between 3d- and 5d-element doping underlines a strong magnetoelastic coupling inherent in the Ir-rich oxides.

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Published in Physical Review B: Condensed Matter and Materials Physics, v. 92, no. 2, article 024425, p. 1-5.

©2015 American Physical Society

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This work was supported by the National Science Foundation via Grant No. DMR-1265162 and China Scholarship Council (J.C.W.).

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