Spin splitting of dopant edge state in magnetic zigzag graphene nanoribbons

Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena 1 , 2 that have sparked renewed interest in carbon-based spintronics 3 , 4 . Zigzag graphene nanoribbons (ZGNRs)—quasi one-dimensional semiconducting strips of graphene bounded by parall...

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Published inNature (London) Vol. 600; no. 7890; pp. 647 - 652
Main Authors Blackwell, Raymond E., Zhao, Fangzhou, Brooks, Erin, Zhu, Junmian, Piskun, Ilya, Wang, Shenkai, Delgado, Aidan, Lee, Yea-Lee, Louie, Steven G., Fischer, Felix R.
Format Journal Article
LanguageEnglish
Published London Nature Publishing Group UK 23.12.2021
Nature Publishing Group
Subjects
119/118
142/136
639/638/298/920
639/638/542/968
639/766/119/997
639/925/918/1052
Adsorption
Analysis
Antiferromagnetism
Carbon
Chemical properties
Dopants
Electron spin
Electron states
electronic properties and devices
Electronics
Ferromagnetism
First principles
Functional integration
Geometry
Graphene
Graphite - chemistry
Humanities and Social Sciences
Hybridization
Hydrogen
magnetic materials
Magnetic properties
magnetic properties and materials
Magnetics
MATERIALS SCIENCE
Microscopy
multidisciplinary
Nanoribbons
Nanotechnology
Nanotubes, Carbon - chemistry
Nitrogen
Particle spin
scanning probe microscopy
Science
Science (multidisciplinary)
Spectroscopy
Spectrum analysis
Splitting
Structure
Superlattices
Topography
United States
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Abstract Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena 1 , 2 that have sparked renewed interest in carbon-based spintronics 3 , 4 . Zigzag graphene nanoribbons (ZGNRs)—quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges—host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width 1 , 2 , 5 . Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases 6 – 8 and even metallic zero mode bands 9 , the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support 10 – 15 . Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices 15 – 21 . Decoupling spin-polarized edge states using substitutional N-atom dopants along the edges of a zigzag graphene nanoribbon (ZGNR) reveals giant spin splitting of a N-dopant edge state, and supports the predicted emergent magnetic order in ZGNRs.
AbstractList Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena that have sparked renewed interest in carbon-based spintronics. Zigzag graphene nanoribbons (ZGNRs)-quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges-host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width. Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases and even metallic zero mode bands, the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support. Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Finally, our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices.
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena.sup.1,2 that have sparked renewed interest in carbon-based spintronics.sup.3,4. Zigzag graphene nanoribbons (ZGNRs)--quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges--host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width.sup.1,2,5. Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases.sup.6-8 and even metallic zero mode bands.sup.9, the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support.sup.10-15. Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices.sup.15-21.
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena 1 , 2 that have sparked renewed interest in carbon-based spintronics 3 , 4 . Zigzag graphene nanoribbons (ZGNRs)—quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges—host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width 1 , 2 , 5 . Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases 6 – 8 and even metallic zero mode bands 9 , the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support 10 – 15 . Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices 15 – 21 . Decoupling spin-polarized edge states using substitutional N-atom dopants along the edges of a zigzag graphene nanoribbon (ZGNR) reveals giant spin splitting of a N-dopant edge state, and supports the predicted emergent magnetic order in ZGNRs.
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena that have sparked renewed interest in carbon-based spintronics . Zigzag graphene nanoribbons (ZGNRs)-quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges-host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width . Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases and even metallic zero mode bands , the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support . Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices .
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena1,2 that have sparked renewed interest in carbon-based spintronics3,4. Zigzag graphene nanoribbons (ZGNRs)-quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges-host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width1,2,5. Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases6-8 and even metallic zero mode bands9, the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support10-15. Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices15-21.
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena.sup.1,2 that have sparked renewed interest in carbon-based spintronics.sup.3,4. Zigzag graphene nanoribbons (ZGNRs)--quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges--host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width.sup.1,2,5. Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases.sup.6-8 and even metallic zero mode bands.sup.9, the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support.sup.10-15. Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices.sup.15-21. Decoupling spin-polarized edge states using substitutional N-atom dopants along the edges of a zigzag graphene nanoribbon (ZGNR) reveals giant spin splitting of a N-dopant edge state, and supports the predicted emergent magnetic order in ZGNRs.
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena1,2 that have sparked renewed interest in carbon-based spintronics3,4. Zigzag graphene nanoribbons (ZGNRs)-quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges-host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width1,2,5. Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases6-8 and even metallic zero mode bands9, the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support10-15. Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices15-21.Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena1,2 that have sparked renewed interest in carbon-based spintronics3,4. Zigzag graphene nanoribbons (ZGNRs)-quasi one-dimensional semiconducting strips of graphene bounded by parallel zigzag edges-host intrinsic electronic edge states that are ferromagnetically ordered along the edges of the ribbon and antiferromagnetically coupled across its width1,2,5. Despite recent advances in the bottom-up synthesis of GNRs featuring symmetry protected topological phases6-8 and even metallic zero mode bands9, the unique magnetic edge structure of ZGNRs has long been obscured from direct observation by a strong hybridization of the zigzag edge states with the surface states of the underlying support10-15. Here, we present a general technique to thermodynamically stabilize and electronically decouple the highly reactive spin-polarized edge states by introducing a superlattice of substitutional N-atom dopants along the edges of a ZGNR. First-principles GW calculations and scanning tunnelling spectroscopy reveal a giant spin splitting of low-lying nitrogen lone-pair flat bands by an exchange field (~850 tesla) induced by the ferromagnetically ordered edge states of ZGNRs. Our findings directly corroborate the nature of the predicted emergent magnetic order in ZGNRs and provide a robust platform for their exploration and functional integration into nanoscale sensing and logic devices15-21.
Audience Academic
Author Louie, Steven G.
Delgado, Aidan
Brooks, Erin
Piskun, Ilya
Fischer, Felix R.
Zhao, Fangzhou
Zhu, Junmian
Blackwell, Raymond E.
Wang, Shenkai
Lee, Yea-Lee
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  organization: Department of Chemistry, University of California
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  surname: Zhao
  fullname: Zhao, Fangzhou
  organization: Department of Physics, University of California, Materials Sciences Division, Lawrence Berkeley National Laboratory
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  orcidid: 0000-0002-5834-0679
  surname: Brooks
  fullname: Brooks, Erin
  organization: Department of Chemistry, University of California
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  givenname: Junmian
  surname: Zhu
  fullname: Zhu, Junmian
  organization: Department of Chemistry, University of California
– sequence: 5
  givenname: Ilya
  surname: Piskun
  fullname: Piskun, Ilya
  organization: Department of Chemistry, University of California
– sequence: 6
  givenname: Shenkai
  surname: Wang
  fullname: Wang, Shenkai
  organization: Department of Chemistry, University of California
– sequence: 7
  givenname: Aidan
  surname: Delgado
  fullname: Delgado, Aidan
  organization: Department of Chemistry, University of California
– sequence: 8
  givenname: Yea-Lee
  surname: Lee
  fullname: Lee, Yea-Lee
  organization: Department of Physics, University of California
– sequence: 9
  givenname: Steven G.
  orcidid: 0000-0003-0622-0170
  surname: Louie
  fullname: Louie, Steven G.
  email: sglouie@berkeley.edu
  organization: Department of Physics, University of California, Materials Sciences Division, Lawrence Berkeley National Laboratory
– sequence: 10
  givenname: Felix R.
  orcidid: 0000-0003-4723-3111
  surname: Fischer
  fullname: Fischer, Felix R.
  email: ffischer@berkeley.edu
  organization: Department of Chemistry, University of California, Materials Sciences Division, Lawrence Berkeley National Laboratory, Kavli Energy NanoScience Institute at the University of California Berkeley and the Lawrence Berkeley National Laboratory
BackLink https://www.ncbi.nlm.nih.gov/pubmed/34937899$$D View this record in MEDLINE/PubMed
https://www.osti.gov/servlets/purl/1900420$$D View this record in Osti.gov
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ContentType Journal Article
Copyright The Author(s), under exclusive licence to Springer Nature Limited 2021
2021. The Author(s), under exclusive licence to Springer Nature Limited.
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CorporateAuthor Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
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  name: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)
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34937891 - Nature. 2021 Dec;600(7890):613-614
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Snippet Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena 1 , 2 that have sparked renewed interest in...
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena that have sparked renewed interest in...
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena.sup.1,2 that have sparked renewed interest in...
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena1,2 that have sparked renewed interest in...
Spin-ordered electronic states in hydrogen-terminated zigzag nanographene give rise to magnetic quantum phenomena that have sparked renewed interest in...
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StartPage 647
SubjectTerms 119/118
142/136
639/638/298/920
639/638/542/968
639/766/119/997
639/925/918/1052
Adsorption
Analysis
Antiferromagnetism
Carbon
Chemical properties
Dopants
Electron spin
Electron states
electronic properties and devices
Electronics
Ferromagnetism
First principles
Functional integration
Geometry
Graphene
Graphite - chemistry
Humanities and Social Sciences
Hybridization
Hydrogen
magnetic materials
Magnetic properties
magnetic properties and materials
Magnetics
MATERIALS SCIENCE
Microscopy
multidisciplinary
Nanoribbons
Nanotechnology
Nanotubes, Carbon - chemistry
Nitrogen
Particle spin
scanning probe microscopy
Science
Science (multidisciplinary)
Spectroscopy
Spectrum analysis
Splitting
Structure
Superlattices
Topography
Title Spin splitting of dopant edge state in magnetic zigzag graphene nanoribbons
URI https://link.springer.com/article/10.1038/s41586-021-04201-y
https://www.ncbi.nlm.nih.gov/pubmed/34937899
https://www.proquest.com/docview/2616227945
https://www.proquest.com/docview/2613291195
https://www.osti.gov/servlets/purl/1900420
Volume 600
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