Pressure tuning of the spin-orbit coupled ground state in Sr2IrO4.

X-ray absorption spectroscopy studies of the magnetic-insulating ground state of Sr2IrO4 at ambient pressure show a clear deviation from a strong spin-orbit (SO) limit J(eff)=1/2 state, a result of local exchange interactions and a nonzero tetragonal crystal field mixing SO split J(eff)=1/2, 3/2 states. X-ray magnetic circular dichroism measurements in a diamond anvil cell show a magnetic transition at a pressure of ∼17  GPa, where the "weak" ferromagnetic moment is quenched despite transport measurements showing insulating behavior to at least 40 GPa. The magnetic transition has implications for the origin of the insulating gap and the nature of exchange interactions in this SO coupled system. The expectation value of the angular part of the SO interaction, , extrapolates to zero at ∼80-90  GPa where an increased bandwidth strongly mixes J(eff)=1/2, 3/2 states and SO interactions no longer dominate the electronic ground state of Sr2IrO4.