Data-Driven Discovery of High-Performance Heterobilayer Transition Metal Dichalcogenide-Based Sliding Ferroelectrics

The development of efficient sliding ferroelectric (FE) materials is crucial for advancing next-generation low-power nanodevices. Currently, most efforts focus on homobilayer two-dimensional materials, except for the experimentally reported heterobilayer sliding FE, MoS₂/WS₂. Here, we first screened 870 transition metal dichalcogenide (TMD) bilayer heterostructures derived from experimentally characterized monolayer TMDs and systematically investigated their sliding ferroelectric behavior across various stacking configurations using high-throughput calculations. On the basis of the generated data, we developed an efficient descriptor, named the amplitude of Allen electronegativity difference (Δχ_m), for identifying van der Waals heterobilayers with sliding FE properties. Finally, 16 semiconducting TMD heterobilayers are identified as exhibiting interlayer sliding FE alongside low switching barriers (<21 meV/f.u.), with 10 outperforming the experimental MoS₂/WS₂ system, showing the largest out-of-plane polarization (OPP) values up to 10 times higher than MoS₂/WS₂. These materials exhibit favorable band gaps (0.60-1.80 eV) using the HSE06 method, making them suitable for sliding FE applications. Our findings reveal that polarization switching in these heterobilayers is strongly influenced by the interplay of stacking patterns, material electronegativity, charge transfer, and electronic structures. This study provides a robust framework for designing novel sliding ferroelectric materials and offers a theoretical basis for future experimental research.