Hydrogen Atoms on Zigzag Graphene Nanoribbons: Chemistry and Magnetism Meet at the Edge

Abstract

Although the unconventional $\pi$-magnetism at the zigzag edges of graphene holds promise for a wide array of applications, whether and to what degree it plays a role in their chemistry remains poorly understood. Here, we investigate the addition of a hydrogen atom $-$ the simplest yet the most experimentally relevant adsorbate $-$ to zigzag graphene nanoribbons (ZGNRs). We show that the $\pi$-magnetism governs the chemistry of ZGNRs, giving rise to a site-dependent reactivity of the carbon atoms and driving the hydrogenation process to the nanoribbon edges. Conversely, the chemisorbed hydrogen atom governs the $\pi$-magnetism of ZGNRs, acting as a spin-$\frac{1}{2}$ paramagnetic center in the otherwise antiferromagnetic ground state and spin-polarizing the charge carriers at the band extrema. Our findings establish a comprehensive picture of the peculiar interplay between chemistry and magnetism that emerges at the zigzag edges of graphene.

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• Monolayer C${}_{60}$ networks: A first-principles perspective
• One-Dimensional Moiré Physics and Chemistry in Heterostrained Bilayer Graphene
• Electronic structure of fullerene nanoribbons
• Topological Domain Walls in Graphene Nanoribbons with Carrier Doping
• Tuning magnetism in graphene nanoribbons via strain and adatoms
• Creating quantum spin chains through edge reconstruction in pure graphene armchair nanoribbons towards ballistic spin transport