Magnetic order, disorder, and excitations under pressure in the Mott insulator Sr2IrO4
Abstract
Protected by the interplay of on-site Coulomb interactions and spin-orbit coupling, Sr2IrO4 at high pressure is a rare example of a Mott insulator with a paramagnetic ground state. Here, using optical Raman scattering, we measure both the phonon and magnon evolution in Sr2IrO4 under pressure, and identify three different magnetically-ordered phases, culminating in a spin-disordered state beyond 18 GPa. A strong first-order structural phase transition drives the magnetic evolution at 10 GPa with reduced structural anisotropy in the IrO6 cages, leading to increasingly isotropic exchange interactions between the Heisenberg spins and a spin-flip transition to c-axis-aligned antiferromagnetic order. In the disordered phase of Heisenberg Jeff=1/2 pseudospins, the spin excitations are quasi-elastic and continuous to 10 meV, potentially hosting a gapless quantum spin liquid in Sr2IrO4.
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