Raman Scattering of Spin-Orbit Mott Insulator Sr₂IrO₄ at High-Pressure

The interplays of electron-electron interaction (U), spin-orbit coupling (SOC), and crystal field effects in the 5d transition metal oxides are complex, which can be turned by external fields to induce many novel electromagnetic phenomena and become one of hot topics in condensed matter physics. In this study, the Raman spectroscopy is carried out on single crystals of Sr₂IrO₄ at room temperature. We discover that when pressure reaches 19.6 GPa to 22.2 GPa, a new peak appears at a wavenumber of 199 cm^-1 in the Raman spectra, accompanied with some anomalous changes of other Raman peaks. This result clearly evidences a structural phase transition occurs, although the existence of the such a transition has been long debated. The structural phase transition is independent of the magnetic phase transition at low temperature, but plays a dominant role in the magnetic ordering transition, owing to the strong spin-orbit coupling. This discovery promises a new way tune electromagnetic properties in the 5d Mott insulators and also provides a new idea to design novel functional materials in the future.