Large Photoinduced Tuning of Ferroelectricity in Sliding Ferroelectrics

We use ab initio calculations and demonstrate that in prototype sliding ferroelectrics rhombohedrally-stacked bilayer transition metal dichalcogenides MoS₂, the out-of-plane electric polarization can be robustly tuned by photoexcitation in a large range for a given sliding. Such tuning is associated with both a structural origin—i.e., photoinduced structural distortion—and a charge origin, namely, the distribution of photoexcited carriers. We elucidate different roles that photoexcitation plays in modulating sliding ferroelectricity under different light intensities, and we highlight the pivotal role of light in manipulating polarization of 2D vdW materials.

We acknowledge the support from the Grant No. MURI ETHOS W911NF-21-2-0162 from Army Research Office (ARO), the ARO Grant No. W911NF-21–1–0113, and the Vannevar Bush Faculty Fellowship (VBFF) Grant No. N00014-20-1-2834 from the Department of Defense. We also acknowledge the computational support from the Naval HPC Pathfinder award for computational resources and from the Arkansas High Performance Computing Center.