• • Twist-angle-dependent polar vortex textures in bilayer MoS2 range from intricate vortex patterns to twelve-fold quasicrystal polar domains, with chiral features (clockwise in AB, anti-clockwise in BA regions) observed via 4D-STEM, enabling precise control of polarization at the picometer scale for nanoscale ferroelectric devices.
• • At a twist angle of 30°, the bilayer MoS2 exhibits an incommensurate quasicrystal structure with 12-fold rotational symmetry, producing rich polar vortex patterns that can be manipulated via interlayer sliding at the picometer scale, offering a pathway for ultrahigh-density data storage with potential bit sizes below 1 nm².
• • First-principles calculations attribute the in-plane polar vortex domains primarily to twist-induced interfacial charge redistribution, with a minor contribution from in-plane ionic displacements, providing a design rule for engineering polarization in non-ferroelectric 2D materials without external fields.
• • The correlation between local atomic structures and 3D spatial electric field distributions, established through combined 4D-STEM and theoretical calculations, enables deterministic control of topological polarization structures, critical for developing low-power topological electronics and neuromorphic computing architectures.