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Neutron scattering study of correlated phase behavior in Sr2IrO4

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 Added by Stephen Wilson
 Publication date 2012
  fields Physics
and research's language is English




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Neutron diffraction measurements are presented exploring the magnetic and structural phase behaviors of the candidate J$_{eff}=1/2$ Mott insulating iridate Sr$_2$IrO$_4$. Comparisons are drawn between the correlated magnetism in this single layer system and its bilayer analog Sr$_3$Ir$_2$O$_7$ where both materials exhibit magnetic domains originating from crystallographic twinning and comparable moment sizes. Weakly temperature dependent superlattice peaks violating the reported tetragonal space group of Sr$_2$IrO$_4$ are observed supporting the notion of a lower structural symmetry arising from a high temperature lattice distortion, and we use this to argue that moments orient along a unique in-plane axis demonstrating an orthorhombic symmetry in the resulting spin structure. Our results demonstrate that the correlated spin order and structural phase behaviors in both single and bilayer Sr$_{n+1}$Ir$_{n}$O$_{3n+1}$ systems are remarkably similar and suggest comparable correlation strengths in each system.



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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 Neel 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.
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