Embedded Three‐Dimensional Bubble‐Like Polar Textures with Ionic‐Ordering‐Assisted Stabilization in CuInP ₂ S ₆

Bubble‐like polar textures in ferroelectrics offer promising opportunities for high‐density memory and neuromorphic devices, yet their stabilization in intrinsic three‐dimensional (3D) objects remains challenging. Here, we report embedded three‐dimensional bubble‐like polar textures in the van der Waals ferroionic crystal CuInP 2 S 6 (CIPS). By combining angle‐resolved vector piezoresponse force microscopy, tomographic piezoresponse force microscopy, and transmission electron microscopy, we reveal that these polar textures are isolated, capsule‐shaped polar nanostructures volumetrically embedded within the CIPS lattice rather than surface‐localized features. The angle‐dependent piezoresponse is consistent with a center‐divergent Néel‐like polarization configuration, while cross‐sectional microscopy indicates local site‐selective Cu‐ion occupancy within the embedded textures, providing a plausible structural basis for ionic‐ordering‐assisted stabilization. Distinct from interface‐constrained polar textures in conventional oxide heterostructures, these bubble‐like textures exhibit only weak size variation over a broad thickness range, suggesting an intrinsically stabilized, ionic‐ordering‐related origin. Furthermore, they can be reversibly reconfigured between bubble‐like and quasi‐single‐domain states under moderate electric bias, plausibly through local Cu‐ion redistribution. These findings highlight ionic ordering as a promising route for stabilizing and manipulating embedded 3D polar textures in van der Waals ferroics and suggest opportunities for electrically reconfigurable nanoscale ferroic devices.