Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films

Dong Li, Hongguang Wang (), Kaifeng Li, Bonan Zhu (), Kai Jiang (), Dirk Backes, Larissa S. I. Veiga, Jueli Shi, Pinku Roy, Ming Xiao, Aiping Chen, Quanxi Jia, Tien-Lin Lee, Sarnjeet S. Dhesi, David O. Scanlon, Judith L. MacManus-Driscoll, Peter A. Aken, Kelvin H. L. Zhang () and Weiwei Li ()
Additional contact information
Dong Li: Nanjing University of Aeronautics and Astronautics
Hongguang Wang: Max Planck Institute for Solid State Research
Kaifeng Li: Nanjing University of Aeronautics and Astronautics
Bonan Zhu: University College London
Kai Jiang: East China Normal University
Dirk Backes: Harwell Science and Innovation Campus
Larissa S. I. Veiga: Harwell Science and Innovation Campus
Jueli Shi: Xiamen University
Pinku Roy: Los Alamos National Laboratory
Ming Xiao: University of Cambridge
Aiping Chen: Los Alamos National Laboratory
Quanxi Jia: University at Buffalo-The State University of New York
Tien-Lin Lee: Harwell Science and Innovation Campus
Sarnjeet S. Dhesi: Harwell Science and Innovation Campus
David O. Scanlon: University College London
Judith L. MacManus-Driscoll: University of Cambridge
Peter A. Aken: Max Planck Institute for Solid State Research
Kelvin H. L. Zhang: Xiamen University
Weiwei Li: Nanjing University of Aeronautics and Astronautics

Nature Communications, 2023, vol. 14, issue 1, 1-9

Abstract: Abstract Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be effectively engineered by strain, defects, and microstructure. An excellent example can be found in ferroelastic LaCoO3 with paramagnetism in bulk. In contrast, unexpected ferromagnetism is observed in tensile-strained LaCoO3 films, however, its origin remains controversial. Here we simultaneously reveal the formation of ordered oxygen vacancies and previously unreported long-range suppression of CoO6 octahedral rotations throughout LaCoO3 films. Supported by density functional theory calculations, we find that the strong modification of Co 3d-O 2p hybridization associated with the increase of both Co-O-Co bond angle and Co-O bond length weakens the crystal-field splitting and facilitates an ordered high-spin state of Co ions, inducing an emergent ferromagnetic-insulating state. Our work provides unique insights into underlying mechanisms driving the ferromagnetic-insulating state in tensile-strained ferroelastic LaCoO3 films while suggesting potential applications toward low-power spintronic devices.

Date: 2023
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DOI: 10.1038/s41467-023-39369-6

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