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Spin-Delocalization with a Twist: Chiral Open-Shell Helices

Periodic Reporting for period 4 - INSPIRAL (Spin-Delocalization with a Twist: Chiral Open-Shell Helices)

Période du rapport: 2021-10-01 au 2023-03-31

INSPIRAL addresses the challenge of controlling magnetism and conductivity in all-organic materials based on graphene that are foreseen to revolutionize nanoelectronics and information technology. Their main advantages over other materials like inorganic compounds and metals are flexibility, light weight, and easy processability using solution-based techniques, which makes them suitable for large-scale production and low-cost printing.

Since its discovery by mechanical exfoliation from graphite, a two-dimensional material 'graphene' and its structurally defined molecular fragments, 'nanographenes', have been the focus of intense research. Among many of their exceptional features, magnetism is displayed only by one class of these materials – the so-called open-shell nanographenes. These organic π-radicals feature multiple unpaired electrons and these are responsible for their magnetic properties. Open-shell nanographenes are envisioned as promising future materials because spin interactions between the unpaired electrons provide a unique platform for controlling quantum information or inducing magnetism, which can enable transition of the traditional electronics to “spintronics”. INSPIRAL addresses the challenge of controlling spin interactions in these materials by developing molecular systems, where spin interactions can be tuned within a single molecule to understand the principles that govern an intermolecular assembly in the solid state and their bulk properties. Such level of control will give rise to stimuli-responsive self-assembled materials, in which bulk magnetic and conducting properties can be tuned by molecular design.
INSPIRAL delivered various synthetic methodologies to access valuable model compounds and to study spin communication between unpaired electrons comprised within these molecular systems. Two types of model systems were realized: fully fused systems in which electrons communicate through the molecular skeleton and space at the same time as well as dynamic systems in which electrons communicate only through space. This project delivered important fundamental insights which can be applied as a tool to control magnetic and conducting properties of nanographene materials via molecular design. In addition, unprecedented reactivity of some of the studied systems was identified, which opens up possibility to exploit these systems as a synthetic tool towards more complex molecular architectures. The results were disseminated by means of peer-reviewed publications (21 in total) and presentations at international conferences or institutions (>50 in total).
INSPIRAL delivered important fundamental knowledge for conceptualizing new ways of creating function using unpaired electrons as 'spin carriers' and realizing new organic materials to advance nanoelectronics and information technology. The most significant results include the know-how for tuning magnetic properties of open-shell nanographenes via through-space interactions and the principle for designing metal-free all-organic magnetic switches.
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