High-throughput exfoliation of multiferroic ternary oxide monolayers with high transition temperature and giant spin splitting

Two-dimensional (2D) non-van der Waals (non-vdW) materials has garnered significant attention in recent years, driven by the remarkable properties inherent in their parent bulk. However, a comprehensive high-throughput exfoliation strategy for non-vdW materials remains unestablished. In this study, we propose a bond density and binding strength criterion to identify exfoliable crystallographic planes in ABO3 compounds, realizing massive exfoliation of ABO3 monolayers with exfoliation energies as low as 0.049 $$\text{eV}/{{\rm{\mathring{\rm A} }}}^{2}$$. We screened 35 stable ABO3 monolayers, which not only harbor diverse multiferroic orders, but also possess intriguing physical properties, such as high Néel/Curie temperature, giant spin splitting (0.606 eV), and wide band gaps (0 − 3.758 eV). The candidates demonstrate tunable band ordering, transition from semiconductor to spin-polarized metal, and switching between antiferromagnetic/ferromagnetic states, with low barrier energy (9.1 meV/atom). Our study builds an approach for the design and discovery of 2D non-vdW monolayers from crystallogrphic planes, offering versatile phase-controlled electronic and spin capabilities and providing new insights into phase manipulation in 2D spintronic devices.