Tailoring Magnetism of Graphene Nanoflakes via Tip-Controlled Dehydrogenation.

Zhao, Chenxiao; Huang, Qiang; Valenta, Leoš; Eimre, Kristjan; Yang, Lin; Yakutovich, Aliaksandr V; Xu, Wangwei; Ma, Ji; Feng, Xinliang; Juríček, Michal; Fasel, Roman; Ruffieux, Pascal; Pignedoli, Carlo A (2024). Tailoring Magnetism of Graphene Nanoflakes via Tip-Controlled Dehydrogenation. Physical review letters, 132(4) American Physical Society 10.1103/PhysRevLett.132.046201

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Atomically precise graphene nanoflakes called nanographenes have emerged as a promising platform to realize carbon magnetism. Their ground state spin configuration can be anticipated by Ovchinnikov-Lieb rules based on the mismatch of π electrons from two sublattices. While rational geometrical design achieves specific spin configurations, further direct control over the π electrons offers a desirable extension for efficient spin manipulations and potential quantum device operations. To this end, we apply a site-specific dehydrogenation using a scanning tunneling microscope tip to nanographenes deposited on a Au(111) substrate, which shows the capability of precisely tailoring the underlying π-electron system and therefore efficiently manipulating their magnetism. Through first-principles calculations and tight-binding mean-field-Hubbard modeling, we demonstrate that the dehydrogenation-induced Au-C bond formation along with the resulting hybridization between frontier π orbitals and Au substrate states effectively eliminate the unpaired π electron. Our results establish an efficient technique for controlling the magnetism of nanographenes.

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