Two-dimensional Heisenberg behavior of J(eff)=1/2 isospins in the paramagnetic state of the spin-orbital Mott insulator Sr2IrO4.

The dynamical correlations of J(eff)=1/2 isospins in the paramagnetic state of spin-orbital Mott insulator Sr2IrO4 were revealed by resonant magnetic x-ray diffuse scattering. We found a two-dimensional antiferromagnetic fluctuation with a large in-plane correlation length exceeding 100 lattice spacings at even 20 K above the magnetic ordering temperature. In marked contrast to the naive expectation of the strong magnetic anisotropy associated with an enhanced spin-orbit coupling, we discovered an isotropic isospin correlation that is well described by the two-dimensional S=1/2 quantum Heisenberg model. The estimated antiferromagnetic coupling constant as large as J∼0.1 eV that is comparable to the small Mott gap (<0.5 eV) points out the weak and marginal Mott character of this spin-orbital entangled system.

Phase-sensitive observation of a spin-orbital Mott state in Sr2IrO4.

Measurement of the quantum-mechanical phase in quantum matter provides the most direct manifestation of the underlying abstract physics. We used resonant x-ray scattering to probe the relative phases of constituent atomic orbitals in an electronic wave function, which uncovers the unconventional Mott insulating state induced by relativistic spin-orbit coupling in the layered 5d transition metal oxide Sr2IrO4. A selection rule based on intra-atomic interference effects establishes a complex spin-orbital state represented by an effective total angular momentum = 1/2 quantum number, the phase of which can lead to a quantum topological state of matter.