Spin splitting of dopant edge state in magnetic zigzag graphene nanoribbons

RE Blackwell, F Zhao, E Brooks, J Zhu, I Piskun… - Nature, 2021 - nature.com
Nature, 2021nature.com
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 …
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. 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, , , , , –.
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