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....

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Main Authors: 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. van Aken, Kelvin H. L. Zhang, Weiwei Li
Format: Article
Language:English
Published: Nature Portfolio 2023-06-01
Series:Nature Communications
Online Access:https://doi.org/10.1038/s41467-023-39369-6
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author 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. van Aken
Kelvin H. L. Zhang
Weiwei Li
author_facet 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. van Aken
Kelvin H. L. Zhang
Weiwei Li
author_sort Dong Li
collection DOAJ
description 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.
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spelling doaj.art-78d790c0d80f4a74b7aba944958b10bb2023-06-25T11:20:53ZengNature PortfolioNature Communications2041-17232023-06-011411910.1038/s41467-023-39369-6Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin filmsDong Li0Hongguang Wang1Kaifeng Li2Bonan Zhu3Kai Jiang4Dirk Backes5Larissa S. I. Veiga6Jueli Shi7Pinku Roy8Ming Xiao9Aiping Chen10Quanxi Jia11Tien-Lin Lee12Sarnjeet S. Dhesi13David O. Scanlon14Judith L. MacManus-Driscoll15Peter A. van Aken16Kelvin H. L. Zhang17Weiwei Li18College 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 AstronauticsMax Planck Institute for Solid State ResearchCollege 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 AstronauticsDepartment of Chemistry, University College LondonDepartment of Materials, East China Normal UniversityDiamond Light Source Ltd., Harwell Science and Innovation CampusDiamond Light Source Ltd., Harwell Science and Innovation CampusState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen UniversityCenter for Integrated Nanotechnologies (CINT), Los Alamos National LaboratoryDepartment of Materials Science and Metallurgy, University of CambridgeCenter for Integrated Nanotechnologies (CINT), Los Alamos National LaboratoryDepartment of Materials Design and Innovation, University at Buffalo-The State University of New YorkDiamond Light Source Ltd., Harwell Science and Innovation CampusDiamond Light Source Ltd., Harwell Science and Innovation CampusDepartment of Chemistry, University College LondonDepartment of Materials Science and Metallurgy, University of CambridgeMax Planck Institute for Solid State ResearchState Key Laboratory of Physical Chemistry of Solid Surfaces, Collaborative Innovation Center of Chemistry for Energy Materials, College of Chemistry and Chemical Engineering, Xiamen UniversityCollege 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 AstronauticsAbstract 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.https://doi.org/10.1038/s41467-023-39369-6
spellingShingle 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. van Aken
Kelvin H. L. Zhang
Weiwei Li
Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
Nature Communications
title Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
title_full Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
title_fullStr Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
title_full_unstemmed Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
title_short Emergent and robust ferromagnetic-insulating state in highly strained ferroelastic LaCoO3 thin films
title_sort emergent and robust ferromagnetic insulating state in highly strained ferroelastic lacoo3 thin films
url https://doi.org/10.1038/s41467-023-39369-6
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