Ting‐Ran Liu, Koushik Jagadish, Xiangwei Guo, Maya Ramesh, Peter Meisenheimer, Harish Kumarasubramanian, Sajid Husain, Ann V. Ngo, Amir Avishai, Jayakanth Ravichandran, Darrell G. Schlom, Ramamoorthy Ramesh, Yu‐Tsun Shao
Nanoscale topological polar textures promise new functionalities for ferroelectric memories and logic, yet their three-dimensional structure and mesoscale organization remain experimentally inaccessible. Here we introduce depth-resolved electron diffraction imaging (DREDI), a fast, non-destructive, method that maps polarization with <50 nm lateral and <10 nm depth sensitivity within fraction of a second. Its high acquisition speed enables the first continuous polarization mapping across six orders of magnitude in length scale, from nanometers to millimeters. Using epitaxial BiFeO3 films, DREDI reveals a hidden depth evolution of polar textures: surface 71˚ stripes evolve into subsurface flux-closure vortices that bifurcate into three-fold vertices near the bottom interface. Cross-sectional multi-slice electron ptychography and phase-field modeling confirm these buried configurations and attribute them to strain heterogeneity and ferroelastic twinning in the SrRuO3 electrode. Large-area analysis further shows that vertex-like frustration forms a mesoscale percolating network above a critical length scale of 4 µm. DREDI enables real-time, volumetric studies of buried topological textures in ferroic nanomaterials. Using newly developed electron imaging and applied to epitaxial BiFeO3 thin films, the authors uncover a depth evolution of polar textures: surface stripe domains transform into subsurface flux-closure vortices, which bifurcate into three-fold vertices near the bottom electrode.