Turning graphene magnetic is a promising challenge to make it an active material for spintronics. Predictions state that graphene structures with specific shapes can spontaneously develop magnetism driven by Coulomb repulsion of π-electrons, but its experimental verification is demanding. Here, we report on the observation and manipulation of individual magnetic moments in graphene open-shell nanostructures on a gold surface. Using scanning tunneling spectroscopy, we detect the presence of single electron spins localized around certain zigzag sites of the carbon backbone via the Kondo effect. We find near-by spins coupled into a singlet ground state and quantify their exchange interaction via singlet-triplet inelastic electron excitations. Theoretical simulations picture how electron correlations result in spin-polarized radical states with the experimentally observed spatial distributions. Extra hydrogen atoms bound to radical sites quench their magnetic moment and switch the spin of the nanostructure in half-integer amounts. Our work demonstrates the intrinsic π-paramagnetism of graphene nanostructures.
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http://dx.doi.org/10.1038/s41467-018-08060-6 | DOI Listing |
Chimia (Aarau)
October 2024
Department of Chemistry, University of Zurich, CH-8057 Zurich.
Chemistry has a habit of surprising us. As we dig deeper, sometimes what we find will change the course of our research.
View Article and Find Full Text PDFSmall
October 2024
Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, 117543, Singapore.
Atomically precise open-shell graphene fragments, such as extended peri-acenes, hold significant interest for electronics and spintronics. However, their inherent high reactivity poses challenges for synthesis and application. In this study, a novel approach is introduced: the fusion of a zigzag-edged peri-tetracene with an all-armchair-edged hexa-peri-hexabenzocoronene (HBC) via two shared benzene rings to produce a stable open-shell hydrocarbon, named dibenzo-peri-heptacene (DBPH).
View Article and Find Full Text PDFRSC Adv
October 2024
Institute of Fundamental Physics (AbinitSim Unit ABINITFOT Group), Consejo Superior de Investigaciones Científicas (CSIC) Madrid Spain
Current advances in synthesizing and characterizing atomically precise monodisperse metal clusters (AMCs) at the subnanometer scale have opened up fascinating possibilities in designing new heterogeneous (photo)catalysts as well as functional interfaces between AMCs and biologically relevant molecules. Understanding the nature of AMC-support interactions at molecular-level is essential for optimizing (photo)catalysts performance and designing novel ones with improved properties. Møller-Plesset second-order perturbation theory (MP2) is one of the most cost-efficient single-reference post-Hartree-Fock wave-function-based theories that can be applied to AMC-support interactions considering adequate molecular models of the support, and thus complementing state-of-the-art dispersion-corrected density functional theory.
View Article and Find Full Text PDFAngew Chem Int Ed Engl
September 2024
State Key Laboratory of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, 210023, China.
Helicene diradical derivatives have attracted widespread attentions because of their unique magnetic and chiroptoelectronic properties, however, crystalline and enantiomerically pure forms of helicene diradicals are extremely rare. Herein, we describe the rational design and synthesis of o-quinone functionalized helicene diradicals with crystalline enantiomerical purity. Diradical dianion salt Rac-3K and its enantiomers P/M-3K were obtained by reduction of corresponding precursors Rac-3 and P/M-3 with two equivalent potassium graphite in THF in the presence of (di)benzo-18-crown-6.
View Article and Find Full Text PDFJ Phys Chem Lett
April 2024
Department of Engineering Mechanics, Northwestern Polytechnical University, Xi'an 710072, China.
Triangulene, as a typical open-shell graphene fragment, has attracted widespread attention for nanospintronics, promising to serve as building blocks in spin-logic units. Here, using calculations, we systematically study the laser-induced ultrafast spin-dynamic processes on triangulene nanoflakes, decorated with a transition-metal atom. The results reveal a competition between the induced magnetic center and the carbon edge of the triangulene, resulting in the coexistence of dual spin-density-distribution patterns on such single-magnetic-center systems, thus opening up possibilities of complex spin-dynamic scenarios beyond the spin flip.
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