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Spin-orbit entangled magnetic dipoles, often referred to as pseudospins, provide a new avenue to explore novel magnetism inconceivable in the weak spin-orbit coupling limit, but the nature of their low-energy interactions remains to be understood. We present a comprehensive study of the static magnetism and low-energy pseudospin dynamics in the archetypal spin-orbit Mott insulator Sr2IrO4. We find that in order to understand even basic magnetization measurements, a formerly overlooked in-plane anisotropy is fundamental. In addition to magnetometry, we use neutron diffraction, inelastic neutron scattering and resonant elastic and inelastic x-ray scattering to identify and quantify the interactions that determine the global symmetry of the system and govern the linear responses of pseudospins to external magnetic felds and their low-energy dynamics. We find that a pseudospin-only Hamiltonian is insufficient for an accurate description of the magnetism in Sr2IrO4 and that pseudospin-lattice coupling is essential. This finding should be generally applicable to other pseudospin systems with sizable orbital moments sensitive to anisotropic crystalline environments.
$rm Sr_2IrO_4$ is an archetypal spin-orbit-coupled Mott insulator and has been extensively studied in part because of a wide range of predicted novel states. Limited experimental characterization of these states thus far brings to light the extraordi
We investigated electronic structure of 5d transition-metal oxide Sr2IrO4 using angle-resolved photoemission, optical conductivity, and x-ray absorption measurements and first-principles band calculations. The system was found to be well described by
High quality epitaxial thin films of Jeff=1/2 Mott insulator Sr2IrO4 with increasing in-plane tensile strain have been grown on top of SrTiO3(001) substrates. Increasing the in-plane tensile strain up to ~0.3% was observed to drop the c/a tetragonali
The concept of the entanglement between spin and orbital degrees of freedom plays a crucial role in understanding various phases and exotic ground states in a broad class of materials, including orbitally ordered materials and spin liquids. We invest
The intertwined charge, spin, orbital, and lattice degrees of freedom could endow 5d compounds with exotic properties. Current interest is focused on electromagnetic interactions in these materials, whereas the important role of lattice geometry rema