Controlling magnetism and transport at perovskite cobaltite interfaces via strain-tuned oxygen vacancy ordering

Shameek Bose; Manish Sharma; Maria A. Torija; Jeff Walter; Nileena Nandakumaran; John Dewey; Josh Schmitt; Jaume Gazquez; Maria Varela; M. Zhernenkov; Michael R. Fitzsimmons; Haile Ambaye; Valeria Lauter; Ondrej Hovorka; Andreas Berger; Chris Leighton

doi:10.1103/PhysRevMaterials.9.L031402

Controlling magnetism and transport at perovskite cobaltite interfaces via strain-tuned oxygen vacancy ordering

Shameek Bose, Manish Sharma, Maria A. Torija, Jeff Walter, Nileena Nandakumaran, John Dewey, Josh Schmitt, Jaume Gazquez, Maria Varela, M. Zhernenkov, Michael R. Fitzsimmons, Haile Ambaye, Valeria Lauter, Ondrej Hovorka, Andreas Berger, Chris Leighton

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Abstract

Complex oxides such as perovskite cobaltites exhibit rich phenomena at interfaces due to the complex interplay between their structural, defect, electronic, and magnetic degrees of freedom. We study this interplay here in the ferromagnetic metallic cobaltite La1-xSrxCoO3-δ, using specific substrates to vary both the heteroepitaxial strain (compressive vs tensile) and growth orientation ((001) vs (110)). Transmission electron microscopy, electron energy-loss spectroscopy, high-resolution X-ray diffraction, magnetometry, polarized neutron reflectometry, and electronic magnetotransport measurements are applied. Lattice mismatch and growth orientation are found to enable the precise control of interfacial oxygen vacancy ordering in La1-xSrxCoO3-δ, thus dictating strain relaxation and oxygen vacancy depth profiles, in turn controlling thickness-dependent magnetic and electronic properties. In particular, compressive strain and (110) orientations minimize deleterious magnetic/electronic dead layer effects, leading to the optimization of interfacial magnetism and transport. Strain and orientation tuning of oxygen vacancy ordering are thus established as powerful means to control physical properties at cobaltite-based interfaces, relevant to several fields.

Original language	English
Article number	L031402
Journal	Physical Review Materials
Volume	9
Issue number	3
DOIs	https://doi.org/10.1103/PhysRevMaterials.9.L031402
State	Published - Mar 2025

Funding

Acknowledgments. This work was primarily supported by the US Department of Energy through the University of Minnesota (UMN) Center for Quantum Materials, under Grant No. DE-SC0016371. Parts of this work were conducted in the UMN Characterization Facility, which is partially supported by the National Science Foundation through the MRSEC program under DMR-2011401. STEM-EELS measurements were carried out in the former STEM group at Oak Ridge National Laboratory, supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. Work at Los Alamos National Laboratory (LANL) was supported by Basic Energy Sciences, US Department of Energy, under grant DE FG03-87ER-45332. LANL is operated by LANL LLC under DOE Contract DE-AC52-06NA25396. This research also used resources at the Spallation Neutron Source, a Department of Energy Office of Science User Facility operated by Oak Ridge National Laboratory. Work at nanoGUNE was supported by the Spanish Ministry of Science and Innovation under the Maria de Maeztu Units of Excellence Program (Grant No. CEX2020-001038-M) and Project No. PID2021-123943NB-I00 (OPTOMETAMAG). UMN authors acknowledge productive discussions with Javier Garcia Barriocanal.

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Bose, S., Sharma, M., Torija, M. A., Walter, J., Nandakumaran, N., Dewey, J., Schmitt, J., Gazquez, J., Varela, M., Zhernenkov, M., Fitzsimmons, M. R., Ambaye, H., Lauter, V., Hovorka, O., Berger, A., & Leighton, C. (2025). Controlling magnetism and transport at perovskite cobaltite interfaces via strain-tuned oxygen vacancy ordering. Physical Review Materials, 9(3), Article L031402. https://doi.org/10.1103/PhysRevMaterials.9.L031402

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title = "Controlling magnetism and transport at perovskite cobaltite interfaces via strain-tuned oxygen vacancy ordering",

abstract = "Complex oxides such as perovskite cobaltites exhibit rich phenomena at interfaces due to the complex interplay between their structural, defect, electronic, and magnetic degrees of freedom. We study this interplay here in the ferromagnetic metallic cobaltite La1-xSrxCoO3-δ, using specific substrates to vary both the heteroepitaxial strain (compressive vs tensile) and growth orientation ((001) vs (110)). Transmission electron microscopy, electron energy-loss spectroscopy, high-resolution X-ray diffraction, magnetometry, polarized neutron reflectometry, and electronic magnetotransport measurements are applied. Lattice mismatch and growth orientation are found to enable the precise control of interfacial oxygen vacancy ordering in La1-xSrxCoO3-δ, thus dictating strain relaxation and oxygen vacancy depth profiles, in turn controlling thickness-dependent magnetic and electronic properties. In particular, compressive strain and (110) orientations minimize deleterious magnetic/electronic dead layer effects, leading to the optimization of interfacial magnetism and transport. Strain and orientation tuning of oxygen vacancy ordering are thus established as powerful means to control physical properties at cobaltite-based interfaces, relevant to several fields.",

author = "Shameek Bose and Manish Sharma and Torija, {Maria A.} and Jeff Walter and Nileena Nandakumaran and John Dewey and Josh Schmitt and Jaume Gazquez and Maria Varela and M. Zhernenkov and Fitzsimmons, {Michael R.} and Haile Ambaye and Valeria Lauter and Ondrej Hovorka and Andreas Berger and Chris Leighton",

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Bose, S, Sharma, M, Torija, MA, Walter, J, Nandakumaran, N, Dewey, J, Schmitt, J, Gazquez, J, Varela, M, Zhernenkov, M, Fitzsimmons, MR, Ambaye, H , Lauter, V, Hovorka, O, Berger, A & Leighton, C 2025, 'Controlling magnetism and transport at perovskite cobaltite interfaces via strain-tuned oxygen vacancy ordering', Physical Review Materials, vol. 9, no. 3, L031402. https://doi.org/10.1103/PhysRevMaterials.9.L031402

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T1 - Controlling magnetism and transport at perovskite cobaltite interfaces via strain-tuned oxygen vacancy ordering

AU - Bose, Shameek

AU - Sharma, Manish

AU - Torija, Maria A.

AU - Walter, Jeff

AU - Nandakumaran, Nileena

AU - Dewey, John

AU - Schmitt, Josh

AU - Gazquez, Jaume

AU - Varela, Maria

AU - Zhernenkov, M.

AU - Fitzsimmons, Michael R.

AU - Ambaye, Haile

AU - Lauter, Valeria

AU - Hovorka, Ondrej

AU - Berger, Andreas

AU - Leighton, Chris

PY - 2025/3

Y1 - 2025/3

N2 - Complex oxides such as perovskite cobaltites exhibit rich phenomena at interfaces due to the complex interplay between their structural, defect, electronic, and magnetic degrees of freedom. We study this interplay here in the ferromagnetic metallic cobaltite La1-xSrxCoO3-δ, using specific substrates to vary both the heteroepitaxial strain (compressive vs tensile) and growth orientation ((001) vs (110)). Transmission electron microscopy, electron energy-loss spectroscopy, high-resolution X-ray diffraction, magnetometry, polarized neutron reflectometry, and electronic magnetotransport measurements are applied. Lattice mismatch and growth orientation are found to enable the precise control of interfacial oxygen vacancy ordering in La1-xSrxCoO3-δ, thus dictating strain relaxation and oxygen vacancy depth profiles, in turn controlling thickness-dependent magnetic and electronic properties. In particular, compressive strain and (110) orientations minimize deleterious magnetic/electronic dead layer effects, leading to the optimization of interfacial magnetism and transport. Strain and orientation tuning of oxygen vacancy ordering are thus established as powerful means to control physical properties at cobaltite-based interfaces, relevant to several fields.

AB - Complex oxides such as perovskite cobaltites exhibit rich phenomena at interfaces due to the complex interplay between their structural, defect, electronic, and magnetic degrees of freedom. We study this interplay here in the ferromagnetic metallic cobaltite La1-xSrxCoO3-δ, using specific substrates to vary both the heteroepitaxial strain (compressive vs tensile) and growth orientation ((001) vs (110)). Transmission electron microscopy, electron energy-loss spectroscopy, high-resolution X-ray diffraction, magnetometry, polarized neutron reflectometry, and electronic magnetotransport measurements are applied. Lattice mismatch and growth orientation are found to enable the precise control of interfacial oxygen vacancy ordering in La1-xSrxCoO3-δ, thus dictating strain relaxation and oxygen vacancy depth profiles, in turn controlling thickness-dependent magnetic and electronic properties. In particular, compressive strain and (110) orientations minimize deleterious magnetic/electronic dead layer effects, leading to the optimization of interfacial magnetism and transport. Strain and orientation tuning of oxygen vacancy ordering are thus established as powerful means to control physical properties at cobaltite-based interfaces, relevant to several fields.

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Controlling magnetism and transport at perovskite cobaltite interfaces via strain-tuned oxygen vacancy ordering

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