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Symmetry mismatch has become a topic of immense interest  to those investigating new interfacial phenomena. The interfacial and bulk microstructure of the brownmillerite–perovskite interface is probed using detailed transmission electron microscopy. Unique asymmetric displacements of the tetrahedra at the interface are observed, signifying a compensation mechanism for lattice and symmetry mismatch at the interface.

Symmetry‐Driven Atomic Rearrangement at a Brownmillerite–Perovskite Interface