Decoupling of magnetism and electric transport in single-crystal (Sr_1–xA_x)₂IrO₄ (A = Ca or Ba)

Here, we report a systematical structural, transport and magnetic study of Ca or Ba doped Sr₂IrO₄ single crystals. Isoelectronically substituting Ca²⁺ (up to 15%) or Ba²⁺ (up to 4%) ion for the Sr²⁺ ion provides no additional charge carriers but effectively changes the lattice parameters in Sr₂IrO₄. In particular, 15% Ca doping considerably reduces the c-axis and the unit cell by nearly 0.45% and 1.00%, respectively. These significant, anisotropic compressions in the lattice parameters conspicuously cause no change in the Néel temperature which remains at 240 K, but drastically reduces the electrical resistivity by up to five orders of magnitude or even precipitates a sharp insulator-to-metal transition at lower temperatures, i.e. the vanishing insulating state accompanies an unchanged Néel temperature in (Sr_1–xA_x)₂IrO₄. This observation brings to light an intriguing difference between chemical pressure and applied pressure, the latter of which does suppress the long-range magnetic order in Sr₂IrO₄. This difference reveals the importance of the Ir1–O2–Ir1 bond angle and homogenous volume compression in determining the magnetic ground state. All results, along with a comparison drawn with results of Tb and La doped Sr₂IrO₄, underscore that the magnetic transition plays a nonessential role in the formation of the charge gap in the spin–orbit-tuned iridate.