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
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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 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.
AbstractList	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.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. 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. 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. 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 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.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 LaCoO3 epitaxial films by strain-defect-microstructure manipulated electronic and magnetic states. 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.
ArticleNumber	3638
Author	Shi, Jueli Li, Weiwei Jia, Quanxi Li, Kaifeng Dhesi, Sarnjeet S. Scanlon, David O. Wang, Hongguang Roy, Pinku Jiang, Kai Lee, Tien-Lin Li, Dong Backes, Dirk Chen, Aiping Zhu, Bonan Xiao, Ming Zhang, Kelvin H. L. Veiga, Larissa S. I. MacManus-Driscoll, Judith L. van Aken, Peter A.
Author_xml	– sequence: 1 givenname: Dong surname: Li fullname: Li, Dong organization: College of Physics, MIIT Key Laboratory of Aerospace Information Materials and Physics, State Key Laboratory of Mechanics and Control for Aerospace Structures, Nanjing University of Aeronautics and Astronautics – sequence: 2 givenname: Hongguang orcidid: 0000-0001-8552-2323 surname: Wang fullname: Wang, Hongguang email: hgwang@fkf.mpg.de organization: Max Planck Institute for Solid State Research – sequence: 3 givenname: Kaifeng surname: Li fullname: Li, Kaifeng organization: College of Physics, MIIT Key Laboratory of Aerospace Information Materials and Physics, State Key Laboratory of Mechanics and Control for Aerospace Structures, Nanjing University of Aeronautics and Astronautics – sequence: 4 givenname: Bonan orcidid: 0000-0001-5601-6130 surname: Zhu fullname: Zhu, Bonan email: bonan.zhu@ucl.ac.uk organization: Department of Chemistry, University College London – sequence: 5 givenname: Kai orcidid: 0000-0002-5117-6941 surname: Jiang fullname: Jiang, Kai email: kjiang@ee.ecnu.edu.cn organization: Department of Materials, East China Normal University, School of Arts and Sciences, Shanghai Dianji University – sequence: 6 givenname: Dirk orcidid: 0000-0002-1019-3323 surname: Backes fullname: Backes, Dirk organization: Diamond Light Source Ltd., Harwell Science and Innovation Campus – sequence: 7 givenname: Larissa S. I. surname: Veiga fullname: Veiga, Larissa S. I. organization: Diamond Light Source Ltd., Harwell Science and Innovation Campus – sequence: 8 givenname: Jueli surname: Shi fullname: Shi, Jueli organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 9 givenname: Pinku surname: Roy fullname: Roy, Pinku organization: Center for Integrated Nanotechnologies (CINT), Los Alamos National Laboratory, Department of Materials Design and Innovation, University at Buffalo-The State University of New York – sequence: 10 givenname: Ming surname: Xiao fullname: Xiao, Ming organization: Department of Materials Science and Metallurgy, University of Cambridge – sequence: 11 givenname: Aiping orcidid: 0000-0003-2639-2797 surname: Chen fullname: Chen, Aiping organization: Center for Integrated Nanotechnologies (CINT), Los Alamos National Laboratory – sequence: 12 givenname: Quanxi orcidid: 0000-0002-7683-5202 surname: Jia fullname: Jia, Quanxi organization: Department of Materials Design and Innovation, University at Buffalo-The State University of New York – sequence: 13 givenname: Tien-Lin surname: Lee fullname: Lee, Tien-Lin organization: Diamond Light Source Ltd., Harwell Science and Innovation Campus – sequence: 14 givenname: Sarnjeet S. surname: Dhesi fullname: Dhesi, Sarnjeet S. organization: Diamond Light Source Ltd., Harwell Science and Innovation Campus – sequence: 15 givenname: David O. orcidid: 0000-0001-9174-8601 surname: Scanlon fullname: Scanlon, David O. organization: Department of Chemistry, University College London, Diamond Light Source Ltd., Harwell Science and Innovation Campus – sequence: 16 givenname: Judith L. orcidid: 0000-0003-4987-6620 surname: MacManus-Driscoll fullname: MacManus-Driscoll, Judith L. organization: Department of Materials Science and Metallurgy, University of Cambridge – sequence: 17 givenname: Peter A. orcidid: 0000-0003-1890-1256 surname: van Aken fullname: van Aken, Peter A. organization: Max Planck Institute for Solid State Research – sequence: 18 givenname: Kelvin H. L. orcidid: 0000-0001-9352-6236 surname: Zhang fullname: Zhang, Kelvin H. L. email: kelvinzhang@xmu.edu.cn organization: State Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen University – sequence: 19 givenname: Weiwei orcidid: 0000-0001-5781-5401 surname: Li fullname: Li, Weiwei email: wl337@nuaa.edu.cn organization: College of Physics, MIIT Key Laboratory of Aerospace Information Materials and Physics, State Key Laboratory of Mechanics and Control for Aerospace Structures, Nanjing University of Aeronautics and Astronautics
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Snippet	Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be effectively... Abstract Transition metal oxides are promising candidates for the next generation of spintronic devices due to their fascinating properties that can be...
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SubjectTerms	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
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Title	Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
URI	https://link.springer.com/article/10.1038/s41467-023-39369-6 https://www.proquest.com/docview/2827365566 https://www.proquest.com/docview/2827921228 https://www.osti.gov/servlets/purl/2281521 https://pubmed.ncbi.nlm.nih.gov/PMC10279738 https://doaj.org/article/78d790c0d80f4a74b7aba944958b10bb
Volume	14
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