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<p>The perovskite ABO<sub>3</sub> structure serves as the foundation for diverse functional and quantum materials, yet its applications are hindered by challenges in control of film stoichiometry and the precise construction of interfaces, particularly compared to conventional semiconductors. While a layer-by-layer growth mode is frequently cited, we demonstrate that many transition-metal perovskite oxides self-assemble via an energetically favorable layer-inversion mechanism. This phenomenon can be strategically exploited to fine-tune stoichiometry and surface termination at any point during growth. Layer inversion produces consistent behavior in electron diffraction rocking curves and diffracted-beam intensity oscillations during alternating A- and B-site shuttered growth across various polar and nonpolar surfaces. We introduce a model that accurately interprets these oscillations, enabling an entirely in situ method for precise relative and absolute calibration of multielemental A- and B-site fluxes at the percent level. This approach is successfully applied to the growth of a single-phase high-entropy oxide film.</p>

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A universal method for in situ control of stoichiometry and termination of epitaxial perovskite films

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2025年9月29日

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  • Bruce A. Davidson,
  • Aleksandr Yu. Petrov,
  • Fengmiao Li,
  • Rebecca Pons,
  • Pablo Sosa-Lizama,
  • Hyungki Shin,
  • Chong Liu,
  • Pietro Parisse,
  • Piero Torelli,
  • Georg Cristiani,
  • Y. Eren Suyolcu,
  • Peter A. van Aken,
  • Gennady Logvenov,
  • Gideok Kim,
  • Xiaoxing Xi,
  • Eva Benckiser,
  • Ke Zou

摘要

The perovskite ABO3 structure serves as the foundation for diverse functional and quantum materials, yet its applications are hindered by challenges in control of film stoichiometry and the precise construction of interfaces, particularly compared to conventional semiconductors. While a layer-by-layer growth mode is frequently cited, we demonstrate that many transition-metal perovskite oxides self-assemble via an energetically favorable layer-inversion mechanism. This phenomenon can be strategically exploited to fine-tune stoichiometry and surface termination at any point during growth. Layer inversion produces consistent behavior in electron diffraction rocking curves and diffracted-beam intensity oscillations during alternating A- and B-site shuttered growth across various polar and nonpolar surfaces. We introduce a model that accurately interprets these oscillations, enabling an entirely in situ method for precise relative and absolute calibration of multielemental A- and B-site fluxes at the percent level. This approach is successfully applied to the growth of a single-phase high-entropy oxide film.