Abstract

AbstractOxygen octahedral tilting has been recognized to strongly interact with spin, charge, orbital, and lattice degrees of freedom in perovskite oxides. Here, we observe a strain‐driven stripe‐like morphology of two supertetragonal (monoclinic Cc and Cm) phases in the strained BiFeO3/LaAlO3 thin films. The two supertetragonal phases have a similar giant axial ratio but differences in oxygen pyramid tilting mode. Especially, the competition between polar instability and oxygen pyramid tilting is identified using atomically resolved scanning transmission electron microscopy, leading to the polarization rotation across the phase boundary. In addition, microtwins are observed in the Cc phase. Our findings provide new insights of the coupling between ferroelectric polarization and oxygen pyramid tilting in oxide thin films and will help to design novel phase morphology with desirable ferroelectric polarization and properties for new applications in perovskite oxides.

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