Engineering 2D spin networks by on-surface encapsulation of azafullerene radicals in nanotemplates

Gregor Kladnik, Luca Schio, Gregor Bavdek, Yuri Tanuma, Marion Midden Mavrič, Erik Zupanič, Bastien Anézo, Ioanna K. Sideri, Nikos Tagmatarchis, Jannis Volkmann, Hermann A. Wegner, Andrea Goldoni, Christopher P. Ewels, Alberto Morgante, Luca Floreano, Denis Arčon () and Dean Cvetko ()
Additional contact information
Gregor Kladnik: University of Ljubljana
Luca Schio: Basovizza Area Science Park
Gregor Bavdek: Basovizza Area Science Park
Yuri Tanuma: Jožef Stefan Institute
Marion Midden Mavrič: Jožef Stefan Institute
Erik Zupanič: Jožef Stefan Institute
Bastien Anézo: Jožef Stefan Institute
Ioanna K. Sideri: National Hellenic Research Foundation
Nikos Tagmatarchis: National Hellenic Research Foundation
Jannis Volkmann: Justus Liebig University Giessen
Hermann A. Wegner: Justus Liebig University Giessen
Andrea Goldoni: Elettra Sincrotrone Trieste S.C.p.A.
Christopher P. Ewels: UMR 6502 CNRS, Nantes University
Alberto Morgante: Basovizza Area Science Park
Luca Floreano: Basovizza Area Science Park
Denis Arčon: University of Ljubljana
Dean Cvetko: University of Ljubljana

Nature Communications, 2025, vol. 16, issue 1, 1-10

Abstract: Abstract We present an efficient strategy for on-surface engineering of organic metal-free supramolecular complexes with long-term spin protection. By vacuum deposition of azafullerene (C59N•) monomers on a pre-deposited template layer of [10]cycloparaphenylene ([10]CPP) nanohoops on Au(111) surface we exploit the molecular shape matching between the C59N• and [10]CPP for the azafullerene encapsulation with nanohoops in a guest-host complexation geometry. C59N•⊂[10]CPP supramolecular complexes self-assemble into an extended two-dimensional hexagonal lattice yielding a high density network of stable spin-1/2 radicals. We find compelling evidence for electronic coupling between the guest C59N• and the host [10]CPP in supramolecular species. At the same time, [10]CPP effectively protects the radical state of encapsulated azafullerenes against dimerization and inhibits C59N• coupling to the Au substrate. Azafullerene encapsulation by nanohoops represents a viable realization of molecular spin protection while simultaneously demonstrating exceptional self-assembling properties by which large-scale 2D architectures of molecular spins can be realized.

Date: 2025
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DOI: 10.1038/s41467-024-55521-2

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