Deterministic Switching of Antipolar Variants in Antiferroelectric Membranes

Antiferroelectric (AFE) materials, characterized by their antiparallel dipole alignments, offer distinct ferroic functionalities desirable for high-energy-density storage and next-generation low-power electronic devices. However, the intrinsic degeneracy among antipolar domain variants poses a critical obstacle to their deterministic, nonvolatile control and practical integration into functional architectures. Here, selective and reversible manipulation of AFE domain configurations in freestanding PbZrO₃ membranes via electron beam irradiation are demonstrated. By tailoring the electron beam-induced built-in electric field, controlled writing and erasure of both in-plane and out-of-plane antipolar domain variants are enabled. Complementary phase-field simulations uncover the underlying energetic landscape and domain evolution under varying irradiation conditions, offering mechanistic insight into the observed transformations. These findings demonstrate a promising strategy for domain-level engineering of antiferroelectrics, establishing a generic and programmable approach to deterministically control antipolar ordering in perovskite systems-suggesting a pathway toward controlled, reversible switching of AFE domains in nanoscale oxide architectures.