A first-principles study on the intrinsic asymmetric ferroelectricity of the SrTiO_3-BaTiO_3-CaTiO_3 tricolor superlattice at the nanoscale

摘要

We report a systematic theoretical study on the ferroelectric behavior of ultrathin three-component ferroelectric films, e.g., CaTiO_3- BaTiO_3-SrTiO_3, sandwiched between electrodes. Using first-principles calculations we demonstrate that such structures have intrinsic asymmetric ferroelectricity which is robust even at the nanoscale. In addition, there exists a certain relationship between the polarization directions and geometric stacking sequences of the superlattices. Specifically, the lowest energy states always have polarizations pointing from CaTiO_3 via BaTiO_3 to SrTiO_3, while the sequence in the metastable states is SrTiO_3-BaTiO_3-CaTiO_3. Therefore we were able to distinguish one ferroelectric state from its opposite state by means of their geometric stackings along the polarization directions. Besides this, band alignment analysis reveals that such structures are well behaved at the metal/ferroelectric interface, confirming the credibility and reliability of our first-principles calculation. Our finding may suggest a controllable and unambiguous way to build ferroelectric and multiferroic tunnel junctions.