On-demand nanoengineering of in-plane ferroelectric topologies

Abstract Hierarchical assemblies of ferroelectric nanodomains (or superdomains) can exhibit exotic morphologies that lead to distinct behaviors and functionalities. Controlling these superdomains reliably is critical for realizing new states with desired functional properties. Here, using a biased atomic force microscopy tip we reveal a so-called super-switching mechanism of the in-plane superdomains of a model ferroelectric Pb0.6Sr0.4TiO3, demonstrating that the response of this material is dominated by a superdomain nucleation and super-boundary stabilization process. We show that the scanning-probe’s trajectory is key in stabilizing complex defect states, enabling on-demand formation of intricate center-divergent/convergent and flux-closure polar structures. Correlative piezoresponse force microscopy and optical spectroscopy confirm the topological nature and significant tunability of these emergent structures. The stability of the generated structures, validated by phase-field modeling, suggests potential for reliable multi-state nanodevice architectures, offering an alternative route for creating tunable topological structures in neuromorphic circuits, forging a new frontier in nanolithography for ferroics.