Chenxiao Zhao^1*, Qiang Huang², Leoš Valenta³, Kristjan Eimre¹, Lin Yang², Aliaksandr V. Yakutovich¹, Wangwei Xu¹, Xinliang Feng^2,4, Michal Juríček³, Roman Fasel^1,5, Pascal Ruffieux^1*, Carlo A. Pignedoli^1*

1 Swiss Federal Laboratories for Materials Science and Technology, Dübendorf, Switzerland

2 Faculty of Chemistry and Food Chemistry, and Center for Advancing Electronics Dresden, Technical University of Dresden, Dresden 01062, Germany

3 Department of Chemistry, University of Zurich, Zurich 8057, Switzerland

4 Max Planck Institute of Microstructure Physics, Weinberg 2, Halle 06120, Germany

5 Department of Chemistry, Biochemistry and Pharmaceutical Sciences, University of Bern, Bern 3012, Switzerland

* Corresponding authors emails: chenxiao.zhao@emap.ch, pascal.ruffieux@empa.ch, carlo.pignedoli@empa.ch

DOI10.24435/materialscloud:yh-fj [version v1]

Publication date: May 23, 2024

How to cite this record

Chenxiao Zhao, Qiang Huang, Leoš Valenta, Kristjan Eimre, Lin Yang, Aliaksandr V. Yakutovich, Wangwei Xu, Xinliang Feng, Michal Juríček, Roman Fasel, Pascal Ruffieux, Carlo A. Pignedoli, Tailoring magnetism of graphene nanoflakes via tip-controlled dehydrogenation, Materials Cloud Archive 2024.79 (2024), https://doi.org/10.24435/materialscloud:yh-fj

Description

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, in a recent publication, we applied a site-specific dehydrogenation using a scanning tunneling microscope tip to nanographenes deposited on a Au(111) substrate, which showed the capability of precisely tailoring the underlying π-electron system and therefore efficiently manipulating their magnetism. Through first-principles calculations and tight-binding meanfield-Hubbard modeling, we demonstrated 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. This record contains data that support the scientific results discussed in our manuscript.

Materials Cloud sections using this data

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Keywords

magnetic nanographene CSCS MARVEL/P4 SNSF DFT STM on surface synthesis