Robust spin-orbit coupling in semi-metallic SrIrO3 under hydrostatic pressure

TL;DR

This study investigates the robustness of spin-orbit coupling in SrIrO3 under high pressure, revealing that despite orbital mixing and decreased <LS>, the effective spin-orbit coupling remains stable up to 50 GPa.

Contribution

It demonstrates that the spin-orbit coupled ground state in SrIrO3 is resilient under high hydrostatic pressure, extending understanding of its electronic stability.

Findings

Effective spin-orbit coupling remains stable up to 50 GPa.

Orbital mixing increases with pressure, reducing <LS> by about 15%.

Spectral weight redistribution is due to orbital mixing, not covalency breakdown.

Abstract

The semi-metallic behavior of the perovskite iridate SrIrO3 shifts the end-member of the strongly spin-orbit (SO) coupled Ruddlesden-Popper series Srn+1IrnO3n+1 away from the Mott insulating regime and the half-filled pseudospin Jeff=1/2 ground state well-established in the layered iridates (n = 1 and 2). To investigate the robustness of the SO coupled ground state of SrIrO3, X-ray absorption spectroscopy was carried out at the Ir L2,3 edges under hydrostatic pressure up to 50 GPa at room temperature. The effective SO coupling was deduced from the branching ratio of the Ir L2 and L3 white lines. With increasing pressure, the branching ratio decreases, and the Ir L2,3 peak positions shift to higher energies. The number of 5d holes remains constant indicating that the spectral weight redistribution and peak shifts arise from orbital mixing between t2g and eg related states. The expectation value of the angular part of the SO operator <LS> decreases by about 15% at 50 GPa. This reduction, which is very similar to that observed in the layered iridates, is well explained by an increase of the octahedral crystal field due to the shortening of the Ir-O bond-length under compression. Consistent with theoretical predictions, the orbital mixing and <LS> decrease as the crystal field increases. However, the effective SO coupling remains robust against pressure and does not indicate a covalency-driven breakdown within the investigated pressure range.