Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
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.
- Authors:
-
- Nanjing University of Aeronautics and Astronautics (China)
- Max Planck Institute for Solid State Research, Stuttgart (Germany)
- University College London (United Kingdom)
- East China Normal University, Shanghai (China); Shanghai Dianji University (China)
- Diamond Light Source Ltd., Didcot (United Kingdom)
- Xiamen University (China)
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT); State University of New York at Buffalo, NY (United States)
- University of Cambridge (United Kingdom)
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States). Center for Integrated Nanotechnologies (CINT)
- State University of New York at Buffalo, NY (United States)
- University College London (United Kingdom); Diamond Light Source Ltd., Didcot (United Kingdom)
- Publication Date:
- Research Org.:
- Los Alamos National Laboratory (LANL), Los Alamos, NM (United States)
- Sponsoring Org.:
- USDOE Laboratory Directed Research and Development (LDRD) Program; USDOE National Nuclear Security Administration (NNSA); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF); National Natural Science Foundation of China (NSFC); National Science Foundation (NSF); National Natural Science Foundation of Jiangsu Province; Engineering and Physical Sciences Research Council (EPSRC)
- OSTI Identifier:
- 2281521
- Report Number(s):
- LA-UR-23-30520
Journal ID: ISSN 2041-1723
- Grant/Contract Number:
- 89233218CNA000001; 52102177; 21872116; 22075232; BK20210313; EP/R029431; EP/P020194; ECCS-1902623
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Nature Communications
- Additional Journal Information:
- Journal Volume: 14; Journal Issue: 1; Journal ID: ISSN 2041-1723
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; Material Science
Citation Formats
Li, Dong, Wang, Hongguang, Li, Kaifeng, Zhu, Bonan, Jiang, Kai, Backes, Dirk, Veiga, Larissa S. I., Shi, Jueli, Roy, Pinku, Xiao, Ming, Chen, Aiping, Jia, Quanxi, Lee, Tien-Lin, Dhesi, Sarnjeet S., Scanlon, David O., MacManus-Driscoll, Judith L., van Aken, Peter A., Zhang, Kelvin H. L., and Li, Weiwei. Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films. United States: N. p., 2023.
Web. doi:10.1038/s41467-023-39369-6.
Li, Dong, Wang, Hongguang, Li, Kaifeng, Zhu, Bonan, Jiang, Kai, Backes, Dirk, Veiga, Larissa S. I., Shi, Jueli, Roy, Pinku, Xiao, Ming, Chen, Aiping, Jia, Quanxi, Lee, Tien-Lin, Dhesi, Sarnjeet S., Scanlon, David O., MacManus-Driscoll, Judith L., van Aken, Peter A., Zhang, Kelvin H. L., & Li, Weiwei. Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films. United States. https://doi.org/10.1038/s41467-023-39369-6
Li, Dong, Wang, Hongguang, Li, Kaifeng, Zhu, Bonan, Jiang, Kai, Backes, Dirk, Veiga, Larissa S. I., Shi, Jueli, Roy, Pinku, Xiao, Ming, Chen, Aiping, Jia, Quanxi, Lee, Tien-Lin, Dhesi, Sarnjeet S., Scanlon, David O., MacManus-Driscoll, Judith L., van Aken, Peter A., Zhang, Kelvin H. L., and Li, Weiwei. Mon .
"Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films". United States. https://doi.org/10.1038/s41467-023-39369-6. https://www.osti.gov/servlets/purl/2281521.
@article{osti_2281521,
title = {Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films},
author = {Li, Dong and Wang, Hongguang and Li, Kaifeng and Zhu, Bonan and Jiang, Kai and Backes, Dirk and Veiga, Larissa S. I. and Shi, Jueli and Roy, Pinku and Xiao, Ming and Chen, Aiping and Jia, Quanxi and Lee, Tien-Lin and Dhesi, Sarnjeet S. and Scanlon, David O. and MacManus-Driscoll, Judith L. and van Aken, Peter A. and Zhang, Kelvin H. L. and Li, Weiwei},
abstractNote = {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.},
doi = {10.1038/s41467-023-39369-6},
journal = {Nature Communications},
number = 1,
volume = 14,
place = {United States},
year = {Mon Jun 19 00:00:00 EDT 2023},
month = {Mon Jun 19 00:00:00 EDT 2023}
}
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