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

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. Aken, Gennady Logvenov, Gideok Kim, Xiaoxing Xi, Eva Benckiser () and Ke Zou
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Bruce A. Davidson: University of British Columbia
Aleksandr Yu. Petrov: Area Science Park
Fengmiao Li: University of British Columbia
Rebecca Pons: Max Planck Institute for Solid State Research
Pablo Sosa-Lizama: Max Planck Institute for Solid State Research
Hyungki Shin: University of British Columbia
Chong Liu: University of British Columbia
Pietro Parisse: Area Science Park
Piero Torelli: Area Science Park
Georg Cristiani: Max Planck Institute for Solid State Research
Y. Eren Suyolcu: Max Planck Institute for Solid State Research
Peter A. Aken: Max Planck Institute for Solid State Research
Gennady Logvenov: Max Planck Institute for Solid State Research
Gideok Kim: Max Planck Institute for Solid State Research
Xiaoxing Xi: Temple University
Eva Benckiser: Max Planck Institute for Solid State Research
Ke Zou: University of British Columbia

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract 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.

Date: 2025
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DOI: 10.1038/s41467-025-63608-7

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