Interfacial Strain Gradients Control Nanoscale Domain Morphology in Epitaxial BiFeO3 Multiferroic Films
Résumé
In ferroelectric thin films, the domain structure defines ferroelectric switching pathways and thus influences device performance. In epitaxial bismuth ferrite (BiFeO3) films, fractal-like domains have been observed, but direct evidence of their origins has remained unclear. Here, we show that the nature of the ferroelectric domain structure-i.e. striped vs. fractal-like-in epitaxial BiFeO3 is defined by the strain profile across the film-substrate interface. In samples with fractal-like domains, X-ray diffraction analysis reveals strong strain gradients, while geometric phase analysis using atomic resolution scanning transmission electron microscopy reveals that within a few nanometers of the film-substrate interface, the out of plane strain shows an anomalous dip while the in-plane strain is constant. Electron energy-loss near edge structure at the oxygen K edge shows that in the vicinity of the interface, the oxygen coordination is locally modified; this combined with the anomalous strain behavior thus drives the formation of fractal-like domains. Conversely, if uniform strain is maintained across the interface, characteristic striped domains are formed. Interestingly, conversion from the fractal-like arrangement to striped domains is found possible by an ex-situ thermal treatment step. Critically, the antiferromagnetic state of the BiFeO3 is influenced by the domain structure, whereby the fractal-like domains disrupt the long-range spin cycloid. Finally, as a demonstration of the applicability of this concept, we show that a carefully engineered lower electrode with large strain gradient can be used to induce fractal domains.
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