Room‐Temperature Magnetoelectric Coupling in Strontium Titanate

Abstract Magnetoelectric (ME) multiferroics enable efficient interconversion of electrical and magnetic signals, offering pathways toward substantial reduction of power consumption in next‐generation computing and information technologies. However, despite decades of research, the persistence of ME coupling at room‐temperature, an indispensable feature for practical applications, remains exceedingly rare in single‐phase materials, due to symmetry constraints imposed by magnetic point groups and competing electronic requirements for ferroelectricity and magnetism. Here, the coexistence of ferroelectricity and ferromagnetism is reported at 780 K and a strong ME coupling with a converse ME coupling coefficient up to 498 ps m ⁻¹ at room‐temperature in strontium titanate by dedicated vacancy engineering. The asymmetric distribution of oxygen vacancies surrounding titanium vacancies enables atomic displacement of titanium and charge injection, providing joint origin for ferroelectricity and ferromagnetism, as confirmed by atomic‐scale structural analysis and first‐principles calculations. The mechanism of ME coupling is offered as the hopping of oxygen vacancies under electric fields, which leads to the rearrangement of electronic configuration. This work establishes a novel design paradigm for high‐performance room‐temperature single‐phase multiferroic materials, with particular relevance to perovskite oxide systems.