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

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

doi:10.1016/j.carbon.2020.11.015

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

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 in this paper, 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, andmore » quantum topological properties.« less

Authors:

^[1]; Zhang, Lizhi ^[2];

^[1]; Swett, Jacob L. ^[1];

^[1]; Zhang, Cheng ^[2]; Rack, Philip D. ^[3];

^[3];

^[1];

^[1]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Univ. of Tennessee, Knoxville, TN (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS); Univ. of Tennessee, Knoxville, TN (United States)

Publication Date:: Sat Nov 07 00:00:00 EST 2020

Research Org.:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Org.:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

OSTI Identifier:: 1770656

Alternate Identifier(s):: OSTI ID: 1809387

Grant/Contract Number:: AC05-00OR22725

Resource Type:: Accepted Manuscript

Journal Name:: Carbon

Additional Journal Information:: Journal Volume: 173; Journal ID: ISSN 0008-6223

Publisher:: Elsevier

Country of Publication:: United States

Language:: English

Subject:: 36 MATERIALS SCIENCE; Graphene doping; e-beam manipulation; Magnetic moment; Band gap; Band topology

Citation Formats


                    Dyck, Ondrej, Zhang, Lizhi, Yoon, Mina, Swett, Jacob L., Hensley, Dale K., Zhang, Cheng, Rack, Philip D., Fowlkes, Jason Davidson, Lupini, Andrew R., and Jesse, Stephen. Doping transition-metal atoms in graphene for atomic-scale tailoring of electronic, magnetic, and quantum topological properties.  United States: N. p., 2020. 
Web.  doi:10.1016/j.carbon.2020.11.015.

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                    Dyck, Ondrej, Zhang, Lizhi, Yoon, Mina, Swett, Jacob L., Hensley, Dale K., Zhang, Cheng, Rack, Philip D., Fowlkes, Jason Davidson, Lupini, Andrew R., & Jesse, Stephen. Doping transition-metal atoms in graphene for atomic-scale tailoring of electronic, magnetic, and quantum topological properties.  United States.  https://doi.org/10.1016/j.carbon.2020.11.015

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                    Dyck, Ondrej, Zhang, Lizhi, Yoon, Mina, Swett, Jacob L., Hensley, Dale K., Zhang, Cheng, Rack, Philip D., Fowlkes, Jason Davidson, Lupini, Andrew R., and Jesse, Stephen. Sat .  
"Doping transition-metal atoms in graphene for atomic-scale tailoring of electronic, magnetic, and quantum topological properties".  United States.  https://doi.org/10.1016/j.carbon.2020.11.015.  https://www.osti.gov/servlets/purl/1770656.

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@article{osti_1770656,

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

  author       = {Dyck, Ondrej and Zhang, Lizhi and Yoon, Mina and Swett, Jacob L. and Hensley, Dale K. and Zhang, Cheng and Rack, Philip D. and Fowlkes, Jason Davidson and Lupini, Andrew R. and Jesse, Stephen},

  abstractNote = {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 in this paper, 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.},

  doi          = {10.1016/j.carbon.2020.11.015},

  journal      = {Carbon},

  number       = ,

  volume       = 173,

  place        = {United States},

  year         = {Sat Nov 07 00:00:00 EST 2020},

  month        = {Sat Nov 07 00:00:00 EST 2020}

}

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

Abstract

Citation Formats

Direct Experimental Evidence of Metal-Mediated Etching of Suspended Graphene journal, April 2012

Generalized Gradient Approximation Made Simple journal, October 1996

Graphene spintronics journal, October 2014

Building Structures Atom by Atom via Electron Beam Manipulation journal, August 2018

Mapping mesoscopic phase evolution during E-beam induced transformations via deep learning of atomically resolved images journal, June 2018

Spin qubits in graphene quantum dots journal, February 2007

Stability and Spectroscopy of Single Nitrogen Dopants in Graphene at Elevated Temperatures journal, November 2014

Deep Learning of Atomically Resolved Scanning Transmission Electron Microscopy Images: Chemical Identification and Tracking Local Transformations journal, October 2016

Electron beam-induced formation and displacement of metal clusters on graphene, carbon nanotubes and amorphous carbon journal, January 2012

Observation of the fractional quantum Hall effect in graphene journal, November 2009

Engineering single-atom dynamics with electron irradiation journal, May 2019

Variable voltage electron microscopy: Toward atom-by-atom fabrication in 2D materials journal, April 2020

Quest for magnetism in graphene via Cr- and Mo-doping: A DFT approach journal, April 2016

Fire up the atom forge journal, November 2016

Transition-Metal-Atom-Embedded Graphane and Its Spintronic Device Applications journal, October 2011

A Versatile Common Platform for Quantum Transport Measurements in Fluidic, Cryogenic, and In Situ Electron Microscopy Environments journal, August 2019

Contamination-free graphene by chemical vapor deposition in quartz furnaces journal, August 2017

The electronic properties of graphene journal, January 2009

Stone-Wales-type transformations in carbon nanostructures driven by electron irradiation journal, June 2011

Cleaning graphene: Comparing heat treatments in air and in vacuum: Cleaning graphene journal, July 2017

A spin-filter device based on armchair graphene nanoribbons journal, January 2011

Dynamics of Single Fe Atoms in Graphene Vacancies journal, March 2013

Metal−Graphene Interaction Studied via Atomic Resolution Scanning Transmission Electron Microscopy journal, March 2011

Graphene: New bridge between condensed matter physics and quantum electrodynamics journal, July 2007

Topological band engineering of graphene nanoribbons journal, August 2018

Atomic Mechanisms for the Si Atom Dynamics in Graphene: Chemical Transformations at the Edge and in the Bulk journal, November 2019

Imaging atomic-level random walk of a point defect in graphene journal, May 2014

Exploring the Single Atom Spin State by Electron Spectroscopy journal, November 2015

Two-dimensional gas of massless Dirac fermions in graphene journal, November 2005

Ballistic rectification in a Z-shaped graphene nanoribbon junction journal, March 2008

Migration and Localization of Metal Atoms on Strained Graphene journal, November 2010

Implanting Germanium into Graphene journal, April 2018

Placing single atoms in graphene with a scanning transmission electron microscope journal, September 2017

Colloquium : Andreev reflection and Klein tunneling in graphene journal, October 2008

Perfect spin-filter and spin-valve in carbon atomic chains journal, January 2010

Electric Field Effect in Atomically Thin Carbon Films journal, October 2004

Direct in situ observations of single Fe atom catalytic processes and anomalous diffusion at graphene edges journal, October 2014

Deep learning analysis of defect and phase evolution during electron beam-induced transformations in WS2 journal, February 2019

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set journal, October 1996

Atomic Structure and Dynamics of Metal Dopant Pairs in Graphene journal, June 2014

Learning surface molecular structures via machine vision journal, August 2017

Direct Observation of a Long-Lived Single-Atom Catalyst Chiseling Atomic Structures in Graphene journal, January 2014

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Spintronics and pseudospintronics in graphene and topological insulators journal, April 2012

Doping of Cr in Graphene Using Electron Beam Manipulation for Functional Defect Engineering journal, October 2020

Z-shaped graphene nanoribbon quantum dot device journal, July 2007

Spin and band-gap engineering in doped graphene nanoribbons journal, October 2008

Electron beam nanosculpting of suspended graphene sheets journal, September 2008

Quantum information on chicken wire journal, March 2007

Correlating Atomic Structure and Transport in Suspended Graphene Nanoribbons journal, June 2014

Transition metal adatoms on graphene: A systematic density functional study journal, December 2015

Stability and Dynamics of the Tetravacancy in Graphene journal, February 2014

Inflating Graphene with Atomic Scale Blisters journal, January 2014

In Situ Transmission Electron Microscopy Modulation of Transport in Graphene Nanoribbons journal, April 2016

Quantum dots and spin qubits in graphene journal, July 2010

Embedding Transition-Metal Atoms in Graphene: Structure, Bonding, and Magnetism journal, March 2009

Electronic properties of graphene nanostructures journal, May 2011

Atom-by-atom fabrication with electron beams journal, June 2019

Electronic Structure Modification of Ion Implanted Graphene: The Spectroscopic Signatures of p- and n-Type Doping journal, October 2015

The Role of the Bridging Atom in Stabilizing Odd Numbered Graphene Vacancies journal, June 2014

Probing the Bonding and Electronic Structure of Single Atom Dopants in Graphene with Electron Energy Loss Spectroscopy journal, January 2013

Direct Experimental Evidence of Metal-Mediated Etching of Suspended Graphene
journal, April 2012

Generalized Gradient Approximation Made Simple
journal, October 1996

Graphene spintronics
journal, October 2014

Building Structures Atom by Atom via Electron Beam Manipulation
journal, August 2018

Mapping mesoscopic phase evolution during E-beam induced transformations via deep learning of atomically resolved images
journal, June 2018

Spin qubits in graphene quantum dots
journal, February 2007

Stability and Spectroscopy of Single Nitrogen Dopants in Graphene at Elevated Temperatures
journal, November 2014

Deep Learning of Atomically Resolved Scanning Transmission Electron Microscopy Images: Chemical Identification and Tracking Local Transformations
journal, October 2016

Electron beam-induced formation and displacement of metal clusters on graphene, carbon nanotubes and amorphous carbon
journal, January 2012

Observation of the fractional quantum Hall effect in graphene
journal, November 2009

Engineering single-atom dynamics with electron irradiation
journal, May 2019

Variable voltage electron microscopy: Toward atom-by-atom fabrication in 2D materials
journal, April 2020

Quest for magnetism in graphene via Cr- and Mo-doping: A DFT approach
journal, April 2016

Fire up the atom forge
journal, November 2016

Transition-Metal-Atom-Embedded Graphane and Its Spintronic Device Applications
journal, October 2011

A Versatile Common Platform for Quantum Transport Measurements in Fluidic, Cryogenic, and In Situ Electron Microscopy Environments
journal, August 2019

Contamination-free graphene by chemical vapor deposition in quartz furnaces
journal, August 2017

The electronic properties of graphene
journal, January 2009

Stone-Wales-type transformations in carbon nanostructures driven by electron irradiation
journal, June 2011

Cleaning graphene: Comparing heat treatments in air and in vacuum: Cleaning graphene
journal, July 2017

A spin-filter device based on armchair graphene nanoribbons
journal, January 2011

Dynamics of Single Fe Atoms in Graphene Vacancies
journal, March 2013

Metal−Graphene Interaction Studied via Atomic Resolution Scanning Transmission Electron Microscopy
journal, March 2011

Graphene: New bridge between condensed matter physics and quantum electrodynamics
journal, July 2007

Topological band engineering of graphene nanoribbons
journal, August 2018

Atomic Mechanisms for the Si Atom Dynamics in Graphene: Chemical Transformations at the Edge and in the Bulk
journal, November 2019

Imaging atomic-level random walk of a point defect in graphene
journal, May 2014

Exploring the Single Atom Spin State by Electron Spectroscopy
journal, November 2015

Two-dimensional gas of massless Dirac fermions in graphene
journal, November 2005

Ballistic rectification in a Z-shaped graphene nanoribbon junction
journal, March 2008

Migration and Localization of Metal Atoms on Strained Graphene
journal, November 2010

Implanting Germanium into Graphene
journal, April 2018

Placing single atoms in graphene with a scanning transmission electron microscope
journal, September 2017

Colloquium : Andreev reflection and Klein tunneling in graphene
journal, October 2008

Perfect spin-filter and spin-valve in carbon atomic chains
journal, January 2010

Electric Field Effect in Atomically Thin Carbon Films
journal, October 2004

Direct in situ observations of single Fe atom catalytic processes and anomalous diffusion at graphene edges
journal, October 2014

Deep learning analysis of defect and phase evolution during electron beam-induced transformations in WS2
journal, February 2019

Efficient iterative schemes for ab initio total-energy calculations using a plane-wave basis set
journal, October 1996

Atomic Structure and Dynamics of Metal Dopant Pairs in Graphene
journal, June 2014

Learning surface molecular structures via machine vision
journal, August 2017

Direct Observation of a Long-Lived Single-Atom Catalyst Chiseling Atomic Structures in Graphene
journal, January 2014

Building and exploring libraries of atomic defects in graphene: Scanning transmission electron and scanning tunneling microscopy study
journal, September 2019

Spintronics and pseudospintronics in graphene and topological insulators
journal, April 2012

Doping of Cr in Graphene Using Electron Beam Manipulation for Functional Defect Engineering
journal, October 2020

Z-shaped graphene nanoribbon quantum dot device
journal, July 2007

Spin and band-gap engineering in doped graphene nanoribbons
journal, October 2008

Electron beam nanosculpting of suspended graphene sheets
journal, September 2008

Quantum information on chicken wire
journal, March 2007

Correlating Atomic Structure and Transport in Suspended Graphene Nanoribbons
journal, June 2014

Transition metal adatoms on graphene: A systematic density functional study
journal, December 2015

Stability and Dynamics of the Tetravacancy in Graphene
journal, February 2014

Inflating Graphene with Atomic Scale Blisters
journal, January 2014

In Situ Transmission Electron Microscopy Modulation of Transport in Graphene Nanoribbons
journal, April 2016

Quantum dots and spin qubits in graphene
journal, July 2010

Embedding Transition-Metal Atoms in Graphene: Structure, Bonding, and Magnetism
journal, March 2009

Electronic properties of graphene nanostructures
journal, May 2011

Atom-by-atom fabrication with electron beams
journal, June 2019

Electronic Structure Modification of Ion Implanted Graphene: The Spectroscopic Signatures of p- and n-Type Doping
journal, October 2015

The Role of the Bridging Atom in Stabilizing Odd Numbered Graphene Vacancies
journal, June 2014

Probing the Bonding and Electronic Structure of Single Atom Dopants in Graphene with Electron Energy Loss Spectroscopy
journal, January 2013