Pressure-Induced Metal-Insulator and Paramagnet-Altermagnet Transitions in Rutile OsO2 Single Crystals

Abstract

Altermagnets with compensated spin structures and nonrelativistic spin splitting have emerged as a new class of magnetic materials. Rutile OsO2 has been theoretically predicted to be altermagnetic, but experimental studies have been limited by synthesis challenges. We have succeeded in synthesizing high-quality single crystals of rutile OsO2. Electrical transport studies reveal that OsO2 is highly conductive and exhibits clear Fermi liquid behavior, indicating strong electron-electron scattering. Magnetic measurements show that the crystals are isotropically paramagnetic. Density-functional theory calculations indicate that bulk OsO2 is semimetallic with coexisting electron and hole pockets, with its magnetic ground state strongly dependent on the on-site Coulomb correlation U. Angle-resolved photoemission spectroscopy studies unveil that the bulk bands do not yet show altermagnetic spin splitting. Interestingly, resistivity is rather pressure sensitive: at 44 GPa, a clear metal-insulator transition occurs. Hybrid functional calculations reveal that applying pressure significantly increases the Hubbard U value, driving a phase transition from a paramagnetic metal to an altermagnetic metal, and eventually to an altermagnetic insulator. These findings suggest that tuning external pressure effectively modulates the magnetic ground state of OsO2, providing a pathway to realize altermagnetism in this material.