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Non-covalent control of spin-state in metal-organic complex by positioning on N-doped graphene.

Research paper by Bruno B de la Torre, Martin M Švec, Prokop P Hapala, Jesus J Redondo, Ondřej O Krejčí, Rabindranath R Lo, Debashree D Manna, Amrit A Sarmah, Dana D Nachtigallová, Jiří J Tuček, Piotr P Błoński, Michal M Otyepka, Radek R Zbořil, Pavel P Hobza, Pavel P Jelínek

Indexed on: 22 Jul '18Published on: 22 Jul '18Published in: Nature communications



Abstract

Nitrogen doping of graphene significantly affects its chemical properties, which is particularly important in molecular sensing and electrocatalysis applications. However, detailed insight into interaction between N-dopant and molecules at the atomic scale is currently lacking. Here we demonstrate control over the spin state of a single iron(II) phthalocyanine molecule by its positioning on N-doped graphene. The spin transition was driven by weak intermixing between orbitals with z-component of N-dopant (p of N-dopant) and molecule (d, d, d) with subsequent reordering of the Fe d-orbitals. The transition was accompanied by an electron density redistribution within the molecule, sensed by atomic force microscopy with CO-functionalized tip. This demonstrates the unique capability of the high-resolution imaging technique to discriminate between different spin states of single molecules. Moreover, we present a method for triggering spin state transitions and tuning the electronic properties of molecules through weak non-covalent interaction with suitably functionalized graphene.