Title: Spin splitting of dopant edge state in magnetic zigzag graphene nanoribbons

Abstract

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 sensingmore » and logic devices.« less

Authors:

Blackwell, Raymond E. ^[1]; Zhao, Fangzhou ^[2]; Brooks, Erin  ^[1];

• Search DOE PAGES for author "Brooks, Erin"
• Search DOE PAGES for ORCID "0000-0002-5834-0679"

Zhu, Junmian ^[1]; Piskun, Ilya ^[1]; Wang, Shenkai ^[1]; Delgado, Aidan ^[1]; Lee, Yea-Lee ^[1]; Louie, Steven G.  ^[2];

• Search DOE PAGES for author "Louie, Steven G."
• Search DOE PAGES for ORCID "0000-0003-0622-0170"

Fischer, Felix R.  ^[3]

• Search DOE PAGES for author "Fischer, Felix R."
• Search DOE PAGES for ORCID "0000-0003-4723-3111"

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+ Show Author Affiliations

1. Univ. of California, Berkeley, CA (United States)
2. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States); Kavli Energy NanoScience Institute, Berkeley, CA (United States)

Publication Date:

Wed Dec 22 00:00:00 EST 2021

Research Org.:

Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States). National Energy Research Scientific Computing Center (NERSC)

Sponsoring Org.:

USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division; US Department of the Navy, Office of Naval Research (ONR); National Science Foundation (NSF); Center for Energy Efficient Electronics Science; National Institutes of Health (NIH)

OSTI Identifier:

1900420

Grant/Contract Number:  

AC02-05CH11231; N00014-19-1-2503; DMR-1839098; DMR-1926004; ECCS-0939514; N00014-16-1-2921; DGE-11064000; S10OD024998

Resource Type:

Accepted Manuscript

Journal Name:

Nature (London)

Additional Journal Information:

Journal Name: Nature (London); Journal Volume: 600; Journal Issue: 7890; Journal ID: ISSN 0028-0836

Publisher:

Nature Publishing Group

Country of Publication:

United States

Language:

English

Subject:

36 MATERIALS SCIENCE; electronic properties and devices; magnetic materials; magnetic properties and materials; scanning probe microscopy