Title: Fortuitous partners of antiferromagnetic and Mott states in spin-orbit-coupled Sr2IrO4: A study of Sr2Ir1-xMxO4 (M=Fe or Co)

Abstract: Sr2IrO4 is an archetypal spin-orbit-coupled Mott insulator with an antiferromagnetic state below 240 K. Here we report results of our study on single crystals of Sr2Ir1-xFexO4 (0<x<0.32) and Sr2Ir1-xCoxO4 (0<x<0.22). Fe doping retains the antiferromagnetic state but simultaneously precipitates an emergent metallic state whereas Co doping causes a rapid collapse of both the antiferromagnetic and Mott states, giving rise to a confined metallic state featuring a pronounced linearity of the basal-plane resistivity up to 700 K. The results indicate tetravalent Fe4+(3d4) ions in the intermediate spin state with S=1 and Co4+(3d5) ions in the high spin state with S=5/2 substituting for Ir4+(5d5) ions in Sr2IrO4, respectively. The effective magnetic moment closely tracks the N\'eel temperature as doping increases, suggesting that the spin state of the dopant predominately determines the magnetic properties in doped Sr2IrO4. Furthermore, all relevant properties including charge-carrier density (e.g., 1028/m3), Sommerfeld coefficient (e.g., 19 mJ/mole K2) and Wilson ratio (e.g., 2.6), consistently demonstrates a metallic state that is both robust and highly correlated in the two systems, arising from the percolation of bound states and the weakening of structural distortions. This study strongly suggests that the antiferromagnetic and Mott states merely coexist in a fortuitous manner in Sr2IrO4.