Light‐Induced Mott‐Insulator‐to‐Metal Phase Transition in Ultrathin Intermediate‐Spin Ferromagnetic Perovskite Ruthenates

Light control of emergent quantum phenomena is a widely used external stimulus for quantum materials. Generally, perovskite strontium ruthenate SrRuO3 has an itinerant ferromagnetism with a low-spin state. However, the phase of intermediate-spin (IS) ferromagnetic metallic state has never been seen. Here, by means of UV-light irradiation, a photocarrier-doping-induced Mott-insulator-to-metal phase transition is shown in a few atomic layers of perovskite IS ferromagnetic SrRuO3-δ . This new metastable IS metallic phase can be reversibly regulated due to the convenient photocharge transfer from SrTiO3 substrates to SrRuO3-δ ultrathin films. These dynamical mean-field theory calculations further verify such photoinduced electronic phase transformation, owing to oxygen vacancies and orbital reconstruction. The optical manipulation of charge-transfer finesse is an alternative pathway toward discovering novel metastable phases in strongly correlated systems and facilitates potential light-controlled device applications in optoelectronics and spintronics.