High-pressure insulator-to-metal transition in Sr3Ir2O7 studied by x-ray absorption spectroscopy

High-pressure x-ray absorption spectroscopy was performed at the Ir L3 and L2 absorption edges of Sr3Ir2O7. The branching ratio of white-line intensities continuously decreases with pressure, reflecting a reduction in the angular part of the expectation value of the spin-orbit coupling operator, L · S. Up to the high-pressure structural transition at 53 GPa, this behavior can be explained within a single-ion model, where pressure increases the strength of the cubic crystal field, which suppresses the spin-orbit induced hybridization of Jeff = 3/2 and eg levels. We observe a further reduction of the branching ratio above the structural transition, which cannot be explained within a single-ion model of spin-orbit coupling and cubic crystal fields. This change in L · S in the high-pressure, metallic phase of Sr3Ir2O7 could arise from noncubic crystal fields or a bandwidth-driven hybridization of Jeff = 1/2, 3/2 states and suggests that the electronic ground state significantly deviates from the Jeff = 1/2 limit.