Stacking Two‐Dimensional <scp>MoS₂</scp> van der Waals Photocatalyst for Water Splitting via Vertical Strain and Biaxial Strain

ABSTRACT Inspired by the unique features of two‐dimensional materials, herein, we mainly focus on exploring the bilayer MoS 2 using stacking engineering. Given six different stacking configurations, the AB‐type bilayer MoS 2 could be identified as the most thermodynamically favorable, and its unique built‐in electric field characteristics are beneficial for enhancing photocatalytic water splitting. The stacking‐induced interlayer polarization regulates the electronic properties of photoexcited carriers and significantly suppresses the exciton recombination. The suitable band edge position and appropriate ability of carrier separation as well as transfer render it the candidate for photocatalytic water splitting. Especially, it is effective to tune the related properties including band structures, dipole moment, surface potential difference, dipole‐induced built‐in electric field, and absorption as well as photocatalytic activity via vertical strain and biaxial strain. Our work might provide the guidance for further designing brand novel photocatalytic two‐dimensional materials with distinguished optical absorption and high carrier mobilities.