Electron-beam introduction of heteroatomic Pt–Si structures in graphene

Ondrej Dyck; Cheng Zhang; Philip D. Rack; Jason D. Fowlkes; Bobby Sumpter; Andrew R. Lupini; Sergei V. Kalinin; Stephen Jesse

doi:10.1016/j.carbon.2020.01.042

Electron-beam introduction of heteroatomic Pt–Si structures in graphene

Ondrej Dyck, Cheng Zhang, Philip D. Rack, Jason D. Fowlkes, Bobby Sumpter, Andrew R. Lupini, Sergei V. Kalinin, Stephen Jesse

Research output: Contribution to journal › Article › peer-review

32 Scopus citations

Abstract

Electron-beam (e-beam) manipulation of single dopant atoms in an aberration-corrected scanning transmission electron microscope is emerging as a method for directed atomic motion and atom-by-atom assembly. Until now, the dopant species have been limited to atoms closely matched to carbon in terms of ionic radius and capable of strong covalent bonding with carbon atoms in the graphene lattice. In situ dopant insertion into a graphene lattice has thus far been demonstrated only for Si, which is ubiquitously present as a contaminant in this material. Here, we achieve in situ manipulation of Pt atoms and their insertion into the graphene host matrix using the e-beam deposited Pt on graphene as a host system. We further demonstrate a mechanism for stabilization of the Pt atom, enabled through the formation of Si-stabilized Pt heteroatomic clusters attached to the graphene surface. This study provides evidence toward the universality of the e-beam assembly approach, opening a pathway for exploring cluster chemistry through direct assembly.

Original language	English
Pages (from-to)	750-757
Number of pages	8
Journal	Carbon
Volume	161
DOIs	https://doi.org/10.1016/j.carbon.2020.01.042
State	Published - May 2020

Funding

This work was supported by the U.S. Department of Energy , Office of Science , Basic Energy Sciences , Materials Science and Engineering Division (O.D., A.L., S.V.K, B.S., S.J.) and was performed at the Oak Ridge National Laboratory’s Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility. P.D.R. and J.D.F. acknowledge support for the electron beam induced deposition was provided by the Nanofabrication Research Laboratory at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. CZ acknowledges support from the US Department of Energy (DOE) under Grant No. DOE DE-SC0002136 . This work was supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Materials Science and Engineering Division (O.D. A.L. S.V.K, B.S. S.J.) and was performed at the Oak Ridge National Laboratory's Center for Nanophase Materials Sciences (CNMS), a U.S. Department of Energy, Office of Science User Facility. P.D.R. and J.D.F. acknowledge support for the electron beam induced deposition was provided by the Nanofabrication Research Laboratory at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. CZ acknowledges support from the US Department of Energy (DOE) under Grant No. DOE DE-SC0002136.

Funders	Funder number
Center for Nanophase Materials Sciences
Oak Ridge National Laboratory
Oak Ridge National Laboratory
U.S. Department of Energy	DOE DE-SC0002136
Office of Science
Basic Energy Sciences
Division of Materials Sciences and Engineering

Keywords

Atomic manipulation
Dopant cluster assembly
Dopant insertion
Graphene
Scanning transmission electron microscopy

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10.1016/j.carbon.2020.01.042

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title = "Electron-beam introduction of heteroatomic Pt–Si structures in graphene",

abstract = "Electron-beam (e-beam) manipulation of single dopant atoms in an aberration-corrected scanning transmission electron microscope is emerging as a method for directed atomic motion and atom-by-atom assembly. Until now, the dopant species have been limited to atoms closely matched to carbon in terms of ionic radius and capable of strong covalent bonding with carbon atoms in the graphene lattice. In situ dopant insertion into a graphene lattice has thus far been demonstrated only for Si, which is ubiquitously present as a contaminant in this material. Here, we achieve in situ manipulation of Pt atoms and their insertion into the graphene host matrix using the e-beam deposited Pt on graphene as a host system. We further demonstrate a mechanism for stabilization of the Pt atom, enabled through the formation of Si-stabilized Pt heteroatomic clusters attached to the graphene surface. This study provides evidence toward the universality of the e-beam assembly approach, opening a pathway for exploring cluster chemistry through direct assembly.",

keywords = "Atomic manipulation, Dopant cluster assembly, Dopant insertion, Graphene, Scanning transmission electron microscopy",

author = "Ondrej Dyck and Cheng Zhang and Rack, {Philip D.} and Fowlkes, {Jason D.} and Bobby Sumpter and Lupini, {Andrew R.} and Kalinin, {Sergei V.} and Stephen Jesse",

note = "Publisher Copyright: {\textcopyright} 2020",

year = "2020",

month = may,

doi = "10.1016/j.carbon.2020.01.042",

language = "English",

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AU - Dyck, Ondrej

AU - Zhang, Cheng

AU - Rack, Philip D.

AU - Fowlkes, Jason D.

AU - Sumpter, Bobby

AU - Lupini, Andrew R.

AU - Kalinin, Sergei V.

AU - Jesse, Stephen

PY - 2020/5

Y1 - 2020/5

N2 - Electron-beam (e-beam) manipulation of single dopant atoms in an aberration-corrected scanning transmission electron microscope is emerging as a method for directed atomic motion and atom-by-atom assembly. Until now, the dopant species have been limited to atoms closely matched to carbon in terms of ionic radius and capable of strong covalent bonding with carbon atoms in the graphene lattice. In situ dopant insertion into a graphene lattice has thus far been demonstrated only for Si, which is ubiquitously present as a contaminant in this material. Here, we achieve in situ manipulation of Pt atoms and their insertion into the graphene host matrix using the e-beam deposited Pt on graphene as a host system. We further demonstrate a mechanism for stabilization of the Pt atom, enabled through the formation of Si-stabilized Pt heteroatomic clusters attached to the graphene surface. This study provides evidence toward the universality of the e-beam assembly approach, opening a pathway for exploring cluster chemistry through direct assembly.

AB - Electron-beam (e-beam) manipulation of single dopant atoms in an aberration-corrected scanning transmission electron microscope is emerging as a method for directed atomic motion and atom-by-atom assembly. Until now, the dopant species have been limited to atoms closely matched to carbon in terms of ionic radius and capable of strong covalent bonding with carbon atoms in the graphene lattice. In situ dopant insertion into a graphene lattice has thus far been demonstrated only for Si, which is ubiquitously present as a contaminant in this material. Here, we achieve in situ manipulation of Pt atoms and their insertion into the graphene host matrix using the e-beam deposited Pt on graphene as a host system. We further demonstrate a mechanism for stabilization of the Pt atom, enabled through the formation of Si-stabilized Pt heteroatomic clusters attached to the graphene surface. This study provides evidence toward the universality of the e-beam assembly approach, opening a pathway for exploring cluster chemistry through direct assembly.

KW - Atomic manipulation

KW - Dopant cluster assembly

KW - Dopant insertion

KW - Graphene

KW - Scanning transmission electron microscopy

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VL - 161

SP - 750

EP - 757

JO - Carbon

JF - Carbon

ER -

Electron-beam introduction of heteroatomic Pt–Si structures in graphene

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Keywords

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