A universal method for in situ control of stoichiometry and termination of epitaxial perovskite films
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.
Authors
- Xiaoxing Xi (ORCID: https://orcid.org/0000-0002-3808-1358)
- Fengmiao Li (ORCID: https://orcid.org/0000-0001-7729-9432)
- Peter A. van Aken (ORCID: https://orcid.org/0000-0003-1890-1256)
- E. Benckiser (ORCID: https://orcid.org/0000-0002-7638-2282)
- Г. Логвенов (ORCID: https://orcid.org/0000-0003-1986-0249)
- Hyungki Shin (ORCID: https://orcid.org/0000-0001-8435-4479)
- Piero Torelli (ORCID: https://orcid.org/0000-0001-9300-9685)
- Rebecca Pons (ORCID: https://orcid.org/0000-0002-8713-8672)
- Ke Zou (ORCID: https://orcid.org/0000-0002-1181-1779)
- Y. Eren Suyolcu (ORCID: https://orcid.org/0000-0003-0988-5194)
- Gideok Kim (ORCID: https://orcid.org/0000-0003-2667-0064)
- Pietro Parisse (ORCID: https://orcid.org/0000-0002-7420-2778)
- B. A. Davidson (ORCID: https://orcid.org/0000-0003-1616-9380)
- Chong Liu (ORCID: https://orcid.org/0000-0002-2314-8687)
- A. Yu. Petrov (ORCID: https://orcid.org/0000-0002-6199-9319)
- Pablo Sosa-Lizama
- Georg Cristiani
Institutions
- University of British Columbia (CA)
- Max Planck Institute for Solid State Research (DE)
- Istituto Officina dei Materiali (IT)
- Temple University (US)
Publication Details
- Journal
- Nature Communications
- Published
- 2025-09-29
- DOI
- https://doi.org/10.1038/s41467-025-63608-7
- Primary Topic
- Electronic and Structural Properties of Oxides
- Type
- article
- Field-Weighted Citation Impact
- 0.00
Funders
- Gordon and Betty Moore Foundation
- Temple University
- University of Tokyo
- Canada First Research Excellence Fund
- Natural Sciences and Engineering Research Council of Canada