3D oxygen vacancy distribution and defect-property relations in an oxide heterostructure

Kasper A. Hunnestad, Hena Das, Constantinos Hatzoglou, Megan Holtz, Charles M. Brooks, Antonius T. J. Helvoort, David A. Muller, Darrell G. Schlom, Julia A. Mundy and Dennis Meier ()
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Kasper A. Hunnestad: NTNU Norwegian University of Science and Technology
Hena Das: Tokyo Institute of Technology
Constantinos Hatzoglou: NTNU Norwegian University of Science and Technology
Megan Holtz: Cornell University
Charles M. Brooks: Cornell University
Antonius T. J. Helvoort: NTNU Norwegian University of Science and Technology
David A. Muller: Cornell University
Darrell G. Schlom: Cornell University
Julia A. Mundy: Harvard University
Dennis Meier: NTNU Norwegian University of Science and Technology

Nature Communications, 2024, vol. 15, issue 1, 1-6

Abstract: Abstract Oxide heterostructures exhibit a vast variety of unique physical properties. Examples are unconventional superconductivity in layered nickelates and topological polar order in (PbTiO3)n/(SrTiO3)n superlattices. Although it is clear that variations in oxygen content are crucial for the electronic correlation phenomena in oxides, it remains a major challenge to quantify their impact. Here, we measure the chemical composition in multiferroic (LuFeO3)9/(LuFe2O4)1 superlattices, mapping correlations between the distribution of oxygen vacancies and the electric and magnetic properties. Using atom probe tomography, we observe oxygen vacancies arranging in a layered three-dimensional structure with a local density on the order of 1014 cm−2, congruent with the formula-unit-thick ferrimagnetic LuFe2O4 layers. The vacancy order is promoted by the locally reduced formation energy and plays a key role in stabilizing the ferroelectric domains and ferrimagnetism in the LuFeO3 and LuFe2O4 layers, respectively. The results demonstrate pronounced interactions between oxygen vacancies and the multiferroic order in this system and establish an approach for quantifying the oxygen defects with atomic-scale precision in 3D, giving new opportunities for deterministic defect-enabled property control in oxide heterostructures.

Date: 2024
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DOI: 10.1038/s41467-024-49437-0

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