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

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 LaCoO 3 with paramagnetism in bulk. In contr...

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Published in:Nature communications Vol. 14; no. 1; pp. 3638 - 9
Main Authors: 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
Format: Journal Article
Language:English
Published: London Nature Publishing Group UK 19.06.2023
Nature Publishing Group
Nature Portfolio
Subjects:
140/146
147/137
639/301/119/996
639/766/119/996
639/766/119/997
Crystal defects
Density functional theory
Electrons
Ferromagnetic materials
Humanities and Social Sciences
Hybridization
Material Science
MATERIALS SCIENCE
Metal oxides
Microstructure
multidisciplinary
Paramagnetism
Robustness
Science
Science (multidisciplinary)
Thin films
Transition metal oxides
ISSN:2041-1723, 2041-1723
Online Access:Get full text
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Summary: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 LaCoO 3 with paramagnetism in bulk. In contrast, unexpected ferromagnetism is observed in tensile-strained LaCoO 3 films, however, its origin remains controversial. Here we simultaneously reveal the formation of ordered oxygen vacancies and previously unreported long-range suppression of CoO 6 octahedral rotations throughout LaCoO 3 films. Supported by density functional theory calculations, we find that the strong modification of Co 3 d -O 2 p 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 LaCoO 3 films while suggesting potential applications toward low-power spintronic devices. Transition metal oxides are a promising class of materials to engineer multiferroic properties for next-generation spintronic devices. Here, the authors demonstrate an emergent and robust ferromagnetic-insulating state in ferroelastic LaCoO 3 epitaxial films by strain-defect-microstructure manipulated electronic and magnetic states.
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Engineering and Physical Sciences Research Council (EPSRC)
National Natural Science Foundation of Jiangsu Province
USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
LA-UR-23-30520
National Science Foundation (NSF)
89233218CNA000001; 52102177; 21872116; 22075232; BK20210313; EP/R029431; EP/P020194; ECCS-1902623
USDOE Laboratory Directed Research and Development (LDRD) Program
National Natural Science Foundation of China (NSFC)
USDOE National Nuclear Security Administration (NNSA)
ISSN:2041-1723
2041-1723
DOI:10.1038/s41467-023-39369-6