Tailoring Magnetism of Graphene Nanoflakes via Tip-Controlled Dehydrogenation
Chenxiao Zhao, Qiang Huang, Leoš Valenta, Kristjan Eimre, Lin Yang, Aliaksandr V. Yakutovich, Wangwei Xu, Ji Ma, Xinliang Feng, Michal Jurı́ček, Román Fasel, Pascal Ruffieux, Carlo A. Pignedoli
Abstract
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.