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    First-principles study on ferroelectricity in monolayer BaTiO3

    Y. X. Li1, H. Gan1, B. Xu1, H. Y. Zhang1, S. C. Shen1,*, Y. W. Yin1, and X. G. Li1,2,†

    • 1Hefei National Research Center for Physical Sciences at the Microscale, Department of Physics and CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, University of Science and Technology of China, Hefei 230026, China
    • 2Collaborative Innovation Center of Advanced Microstructures, Nanjing University, Nanjing 210093, China

    • *Contact author: scshen@ustc.edu.cn
    • †Contact author: lixg@ustc.edu.cn

    Phys. Rev. B 111, 214114 – Published 20 June, 2025

    DOI: https://doi.org/10.1103/3xqz-pxv5

    Abstract

    Two-dimensional ferroelectricity has garnered significant research interest owing to its potential for enabling novel miniaturized devices. While conventional perovskite ferroelectrics inherently belong to three-dimensional structural systems, preserving robust ferroelectric properties in perovskite-derived structures down to the monolayer limit is important. In this work, we conduct first-principles calculations to systematically investigate the ferroelectricity of BaTiO3 monolayer film, explicitly considering the influences of strain and electrode configuration. For a freestanding BaTiO3 monolayer film with TiO2 termination, in-plane ferroelectricity along the [110] orientation is energetically favored. In the case of a TiO2-terminated BaTiO3 monolayer interfaced with SrRuO3 electrodes, the thermodynamically stable phase undergoes sequential transitions from an in-plane ferroelectric state to a paraelectric intermediate and then to an out-of-plane ferroelectric state, as the in-plane strain varies from tensile to compressive. We further reveal that both electrode and strain significantly modify the Ti-O bond lengths, which plays a crucial role in governing ferroelectric behavior. Besides, even when the thickness of freestanding TiO2-terminated BaTiO3 film reaches eight unit cells, in-plane ferroelectricity along the [110] orientation remains energetically favored under strain-free conditions. However, the out-of-plane antiferroelectric state emerges as the thermodynamically stable state under in-plane compressive strain. Our research contributes to a more comprehensive understanding of ferroelectricity in monolayer perovskite oxides.

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