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.

arXiv commentTo appear in Physical Review B

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• The Challenge of Spin-Orbit-Tuned Ground States in Iridates
• The Jeff=1/2 antiferromagnet Sr2IrO4: A golden avenue toward new physics and functions
• 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${}_4$
• Decoupling of magnetism and electric transport in single-crystal (Sr1-xAx)2IrO4 (A = Ca or Ba)
• Novel Block Excitonic Condensate at $n=3.5$ in a Spin-Orbit Coupled $t_{2g}$ Multiorbital Hubbard Model
• On the electronic ground state of two non-magnetic pentavalent honeycomb iridates
• Electronic and optical properties of La-doped Sr${}_3$Ir${}_2$O${}_7$ epitaxial thin-films
• Possible superconductivity induced by a large spin-orbit coupling in carrier doped iridium oxide insulators: A weak coupling approach
• Sr${}_3$Ir${}_2$O${}_7$F${}_2$: Topochemical conversion of a relativistic Mott state into a spin-orbit driven band insulator
• High-pressure floating zone crystal growth of Sr${}_2$IrO${}_4$
• Structural origin of the Jeff=1/2 antiferromagnetic phase in Ga-doped Sr2IrO4