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    Functional Nanostructured Materials (including low-D carbon)

    Tailoring Electronic and Magnetic Properties of Graphene by Phosphorus Doping
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    • Rostislav Langer
      Rostislav Langer
      Department of Physical Chemistry, Faculty of Science, Palacký University Olomouc, tř. 17 listopadu 12,77146 Olomouc, Czech Republic
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    • , 
    • Piotr Błoński*
      Piotr Błoński
      Regional Centre of Advanced Technologies and Materials, Faculty of Science, Palacký University Olomouc, Šlechtitelů 27, 78371 Olomouc , Czech Republic
      *Email: [email protected]
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      Orcidhttp://orcid.org/0000-0002-7072-232X
    • , 
    • Christoph Hofer
      Christoph Hofer
      Institute for Applied Physics, Eberhard Karls University of Tübingen, Auf der Morgenstelle 10, D-72076 Tübingen, Germany
      Natural and Medical Sciences Institute at the University of Tübingen, Markwiesenstr. 55, D-72770 Reutlingen, Germany
      More by Christoph Hofer
    • , 
    • Petr Lazar
      Petr Lazar
      Regional Centre of Advanced Technologies and Materials, Faculty of Science, Palacký University Olomouc, Šlechtitelů 27, 78371 Olomouc , Czech Republic
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      Orcidhttp://orcid.org/0000-0002-7312-3656
    • , 
    • Kimmo Mustonen
      Kimmo Mustonen
      Faculty of Physics, University of Vienna, Boltzmanngasse 5, A-1090 Vienna, Austria
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      Orcidhttp://orcid.org/0000-0002-0953-7299
    • , 
    • Jannik C. Meyer
      Jannik C. Meyer
      Institute for Applied Physics, Eberhard Karls University of Tübingen, Auf der Morgenstelle 10, D-72076 Tübingen, Germany
      Natural and Medical Sciences Institute at the University of Tübingen, Markwiesenstr. 55, D-72770 Reutlingen, Germany
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      Orcidhttp://orcid.org/0000-0003-4023-0778
    • , 
    • Toma Susi*
      Toma Susi
      Faculty of Physics, University of Vienna, Boltzmanngasse 5, A-1090 Vienna, Austria
      *Email: [email protected]
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      Orcidhttp://orcid.org/0000-0003-2513-573X
    • , and 
    • Michal Otyepka
      Michal Otyepka
      Regional Centre of Advanced Technologies and Materials, Faculty of Science, Palacký University Olomouc, Šlechtitelů 27, 78371 Olomouc , Czech Republic
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      Orcidhttp://orcid.org/0000-0002-1066-5677
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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 30, 34074–34085
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    https://doi.org/10.1021/acsami.0c07564
    Published July 3, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    The electronic and magnetic properties of graphene can be modulated by doping it with other elements, especially those with a different number of valence electrons. In this article, we first provide a three-dimensional reconstruction of the atomic structure of a phosphorus substitution in graphene using aberration-corrected scanning transmission electron microscopy. Turning then to theoretical calculations based on the density functional theory (DFT), we show that doping phosphorus in various bonding configurations can induce magnetism in graphene. Our simulations reveal that the electronic and magnetic properties of P-doped (Gr-P) and/or phosphono-functionalized graphene (Gr-PO3H2) can be controlled by both the phosphorus concentration and configurations, ultimately leading to ferromagnetic (FM) and/or antiferromagnetic (AFM) features with the transition temperature up to room temperature. We also calculate core-level binding energies of variously bonded P to facilitate X-ray photoelectron spectroscopy-based identification of its chemical form present in P-doped graphene-based structures. These results may enable the design of graphene-based organic magnets with tailored properties for future magnetic or spintronic applications.

    Copyright © 2020 American Chemical Society

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    The Supporting Information is available free of charge at https://pubs.acs.org/doi/10.1021/acsami.0c07564.

    • k-point convergence test, scheme for calculating transition temperatures, ΔEFM-AFM and Tc vs distance, comparison of TC obtained using the Ising model for the 3 × 3 cell and the mean-field approach for the 6 × 3 cell, structures, and spin textures; density of state plots, orbital/atom decomposed density of state plots, and Curie temperatures calculated using PBE, SCAN, and PBE0 functionals (PDF)

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    ACS Applied Materials & Interfaces

    Cite this: ACS Appl. Mater. Interfaces 2020, 12, 30, 34074–34085
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acsami.0c07564
    Published July 3, 2020
    Copyright © 2020 American Chemical Society
    Request reuse permissions

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