Large-scale multiferroic complex oxide epitaxy with magnetically switched polarization enabled by solution processing

Complex oxides with tunable structures have many fascinating properties, though high-quality complex oxide epitaxy with precisely controlled composition is still out of reach. Here we have successfully developed solution-based single-crystalline epitaxy for multiferroic (1-x)BiTi_(1-Fe Mg_(1-O₃-(x)CaTiO₃ (BTFM-CTO) solid solution in large area, confirming its ferroelectricity at the atomic scale with strong spontaneous polarization. Careful compositional tuning leads to a bulk magnetization of 0.07 ± 0.035 μ_B/Fe at room temperature, enabling magnetically induced polarization switching exhibiting a large magnetoelectric coefficient of 2.7-3.0 × 10^-7 s/m. This work demonstrates the great potential of solution processing in large-scale complex oxide epitaxy and establishes novel room-temperature magnetoelectric coupling in epitaxial BTFM-CTO film, making it possible to explore a much wider space of composition, phase, and structure that can be easily scaled up for industrial applications.