Doping transition-metal atoms in graphene for atomic-scale tailoring of electronic, magnetic, and quantum topological properties

Ondrej Dyck, Lizhi Zhang, Mina Yoon, Jacob L. Swett, Dale Hensley, Cheng Zhang, Philip D. Rack, Jason D. Fowlkes, Andrew R. Lupini, Stephen Jesse

Research output: Contribution to journalArticlepeer-review

48 Scopus citations

Abstract

Atomic-scale fabrication is an outstanding challenge and overarching goal for the nanoscience community. The practical implementation of moving and fixing atoms to a structure is non-trivial considering that one must spatially address the positioning of single atoms, provide a stabilizing scaffold to hold structures in place, and understand the details of their chemical bonding. Free-standing graphene offers a simplified platform for the development of atomic-scale fabrication and the focused electron beam in a scanning transmission electron microscope can be used to locally induce defects and sculpt the graphene. In this scenario, the graphene forms the stabilizing scaffold and the experimental question is whether a range of dopant atoms can be attached and incorporated into the lattice using a single technique and, from a theoretical perspective, we would like to know which dopants will create technologically interesting properties. Here, we demonstrate that the electron beam can be used to selectively and precisely insert a variety of transition metal atoms into graphene with highly localized control over the doping locations. We use first-principles density functional theory calculations with direct observation of the created structures to reveal the energetics of incorporating metal atoms into graphene and their magnetic, electronic, and quantum topological properties.

Original languageEnglish
Pages (from-to)205-214
Number of pages10
JournalCarbon
Volume173
DOIs
StatePublished - Mar 2021

Funding

Notice to the editor (not to be published): This manuscript has been authored by UT-Battelle, LLC, under Contract No. DE-AC05-00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan (http://energy.gov/downloads/doe-public-access-plan).This material is based upon work supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (O.D. M.Y. A.R.L. S.J.) and Oak Ridge National Laboratory's Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility (D.H. L.Z.). P.D.R. and J.D.F. acknowledge support for the e-beam-induced deposition provided by the Nanofabrication Research Laboratory at CNMS. CZ acknowledges support from the US Department of Energy (DOE) under Grant No. DOE DE-SC0002136. This material is based upon work supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division (O.D., M.Y., A.R.L., S.J.) and Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy , Office of Science User Facility (D.H., L.Z.). P.D.R. and J.D.F. acknowledge support for the e-beam-induced deposition provided by the Nanofabrication Research Laboratory at CNMS. CZ acknowledges support from the US Department of Energy (DOE) under Grant No. DOE DE-SC0002136.

Keywords

  • Band gap
  • Band topology
  • Graphene doping
  • Magnetic moment
  • e-beam manipulation

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