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We demonstrate a route to manipulate the polarization and internal electric field of a complex oxide heterostructure using a layering sequence based on the LaAlO-SrTiO interface. By combining sensitive atomic-level mapping of the structure using direct x-ray phase-retrieval methods with theoretical modeling of the electrostatic charge and polarization, we have devised a novel single-domain polar heterostructure. We find that ionic rearrangement results in strain and free energy minimization, and eliminates the polarization discontinuity leading to a two-fold increase of the spontaneous polarization towards the surface of an ultra-thin single-domain BaTiO film.


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