Structural evolution and electronic properties of (Sr1-xCax)2-yIrO4+z spin-orbit assisted insulators

Abstract

The effect of isoelectronic substitution within single crystals of (Sr1-xCax)2-yIrO4+z is explored. The nominal n=1 Ruddlesden-Popper phase with y=0, z=0 remains stable from x=0 until x=0.11, where the antiferromagnet spin-orbit Mott insulating state persists. An increase in the saturated moment is observed with increasing Ca-substitution, suggesting a modified coupling of the in-plane moments relative to the in-plane rotation of IrO6 octahedra. Beyond x=0.11, the x=1/4, y=0, z=1/2 structural phase Sr3CaIr2O9, consisting of a three-dimensional network of corner sharing octahedra, begins to intermix and eventually nucleates phase pure crystals at higher starting Ca-content. An insulating, nonmagnetic ground state is observed in this phase attributable to the J=0 state and is consistent with a recent powder study. At higher Ca-concentrations beyond x = 0.75, crystals begin to stabilize in the y=1/3, z=0 quasi one-dimensional Ca5Ir3O12 structure. The low temperature transport in this chain-based structure is well described via variable range hopping, and an antiferromagnetic ordering transition appears below T${}_N=9$ K. Our data provide a detailed mapping of the electronic and structural properties accessible as the structural framework of the canonical spin orbit Mott insulator Sr2IrO4 is destabilized via isovalent chemical substitution.

To appear in Physical Review B

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Cited by in corpus (4)

• Optical Signatures of Spin-Orbit Exciton in Bandwidth Controlled Sr${}_2$IrO${}_4$ Epitaxial Films via High-Concentration Ca and Ba Doping
• Magnetism and electrical transport in Y-doped layered iridate Sr${}_2$IrO${}_4$
• Novel Block Excitonic Condensate at $n=3.5$ in a Spin-Orbit Coupled $t_{2g}$ Multiorbital Hubbard Model
• Structural origin of the Jeff=1/2 antiferromagnetic phase in Ga-doped Sr2IrO4