Uncompensated Polarization in Incommensurate Modulations of Perovskite Antiferroelectrics

Complex polar structures of incommensurate modulations (ICMs) are revealed in chemically modified PbZrO3 perovskite antiferroelectrics using advanced transmission electron microscopy techniques. The Pb-cation displacements, previously assumed to arrange in a fully compensated antiparallel fashion, are found to be either antiparallel, but with different magnitudes, or in a nearly orthogonal arrangement in adjacent stripes in the ICMs. Ab initio calculations corroborate the low-energy state of these arrangements. Our discovery corrects the atomic understanding of ICMs in PbZrO3-based perovskite antiferroelectrics.