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

Bruno de la Torre, Martin Švec, Prokop Hapala, Jesus Redondo, Ondřej Krejčí, Rabindranath Lo, Debashree Manna, Amrit Sarmah, Dana Nachtigallová, Jiří Tuček, Piotr Błoński, Michal Otyepka, Radek Zbořil (), Pavel Hobza () and Pavel Jelínek ()
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Bruno de la Torre: Institute of Physics of the Czech Academy of Sciences
Martin Švec: Institute of Physics of the Czech Academy of Sciences
Prokop Hapala: Institute of Physics of the Czech Academy of Sciences
Jesus Redondo: Institute of Physics of the Czech Academy of Sciences
Ondřej Krejčí: Institute of Physics of the Czech Academy of Sciences
Rabindranath Lo: Institute of Organic Chemistry and Biochemistry of the Czech Academy of Sciences
Debashree Manna: Palacký University
Amrit Sarmah: Palacký University
Dana Nachtigallová: Palacký University
Jiří Tuček: Palacký University
Piotr Błoński: Palacký University
Michal Otyepka: Palacký University
Radek Zbořil: Palacký University
Pavel Hobza: Palacký University
Pavel Jelínek: Institute of Physics of the Czech Academy of Sciences

Nature Communications, 2018, vol. 9, issue 1, 1-9

Abstract: 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 (pz of N-dopant) and molecule (dxz, dyz, dz2) 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.

Date: 2018
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DOI: 10.1038/s41467-018-05163-y

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