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Title: Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene

Abstract

Molecules intercalating two-dimensional materials form complex structures that have been characterized primarily by spatially averaged techniques. In this work, we use aberration-corrected scanning transmission electron microscopy and density-functional-theory (DFT) calculations to study the atomic structure of bilayer graphene (BLG) and few-layer graphene (FLG) intercalated with FeC l 3 . In BLG, we discover two distinct intercalated structures that we identify as monolayer FeC l 3 and monolayer FeC l 2 . The two structures are separated by atomically sharp boundaries and induce large free-carrier densities on the order of 1013 c m - 2 in the graphene layers. In FLG, we observe multiple FeC l 3 layers stacked in a variety of possible configurations with respect to one another. Lastly, we find that the microscope's electron beam can convert the FeC l 3 monolayer into FeOCl monolayers in a rectangular lattice. These results reveal the need for a combination of atomically resolved microscopy, spectroscopy, and DFT calculations to identify intercalated structures and study their properties.

Authors:
 [1];  [1];  [2];  [3];  [1];  [4];  [4];  [4];  [5];  [1];  [3];  [1]
+ Show Author Affiliations
  1. Vanderbilt Univ., Nashville, TN (United States)
  2. Vanderbilt Univ., Nashville, TN (United States); Chinese Academy of Sciences (CAS), Beijing (China)
  3. Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  4. Freie Univ., Berlin (Germany)
  5. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
Research Org.:
Vanderbilt Univ., Nashville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Sponsoring Org.:
USDOE Office of Science (SC); National Science Foundation (NSF); European Research Council (ERC)
OSTI Identifier:
1597942
Alternate Identifier(s):
OSTI ID: 1546419
Grant/Contract Number:  
FG02-09ER46554; AC05-00OR22725; ACI-1053575
Resource Type:
Accepted Manuscript
Journal Name:
Physical Review Materials
Additional Journal Information:
Journal Volume: 3; Journal Issue: 6; Journal ID: ISSN 2475-9953
Publisher:
American Physical Society (APS)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY

Citation Formats

Bonacum, Jason P., O’Hara, Andrew, Bao, De-Liang, Ovchinnikov, Oleg S., Zhang, Yan-Fang, Gordeev, Georgy, Arora, Sonakshi, Reich, Stephanie, Idrobo, Juan-Carlos, Haglund, Richard F., Pantelides, Sokrates T., and Bolotin, Kirill I. Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene. United States: N. p., 2019. Web. doi:10.1103/PhysRevMaterials.3.064004.
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Bonacum, Jason P., O’Hara, Andrew, Bao, De-Liang, Ovchinnikov, Oleg S., Zhang, Yan-Fang, Gordeev, Georgy, Arora, Sonakshi, Reich, Stephanie, Idrobo, Juan-Carlos, Haglund, Richard F., Pantelides, Sokrates T., & Bolotin, Kirill I. Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene. United States. https://doi.org/10.1103/PhysRevMaterials.3.064004
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Bonacum, Jason P., O’Hara, Andrew, Bao, De-Liang, Ovchinnikov, Oleg S., Zhang, Yan-Fang, Gordeev, Georgy, Arora, Sonakshi, Reich, Stephanie, Idrobo, Juan-Carlos, Haglund, Richard F., Pantelides, Sokrates T., and Bolotin, Kirill I. Fri . "Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene". United States. https://doi.org/10.1103/PhysRevMaterials.3.064004. https://www.osti.gov/servlets/purl/1597942.
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@article{osti_1597942,
title = {Atomic-resolution visualization and doping effects of complex structures in intercalated bilayer graphene},
author = {Bonacum, Jason P. and O’Hara, Andrew and Bao, De-Liang and Ovchinnikov, Oleg S. and Zhang, Yan-Fang and Gordeev, Georgy and Arora, Sonakshi and Reich, Stephanie and Idrobo, Juan-Carlos and Haglund, Richard F. and Pantelides, Sokrates T. and Bolotin, Kirill I.},
abstractNote = {Molecules intercalating two-dimensional materials form complex structures that have been characterized primarily by spatially averaged techniques. In this work, we use aberration-corrected scanning transmission electron microscopy and density-functional-theory (DFT) calculations to study the atomic structure of bilayer graphene (BLG) and few-layer graphene (FLG) intercalated with FeCl3. In BLG, we discover two distinct intercalated structures that we identify as monolayer FeCl3 and monolayer FeCl2. The two structures are separated by atomically sharp boundaries and induce large free-carrier densities on the order of 1013cm-2 in the graphene layers. In FLG, we observe multiple FeCl3 layers stacked in a variety of possible configurations with respect to one another. Lastly, we find that the microscope's electron beam can convert the FeCl3 monolayer into FeOCl monolayers in a rectangular lattice. These results reveal the need for a combination of atomically resolved microscopy, spectroscopy, and DFT calculations to identify intercalated structures and study their properties.},
doi = {10.1103/PhysRevMaterials.3.064004},
journal = {Physical Review Materials},
number = 6,
volume = 3,
place = {United States},
year = {Fri Jun 28 00:00:00 EDT 2019},
month = {Fri Jun 28 00:00:00 EDT 2019}
}
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Journal Article:
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https://doi.org/10.1103/PhysRevMaterials.3.064004
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Cited by: 8 works
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Figures / Tables:

FIG. 1 FIG. 1: (Left) Diagram of FeCl3-BLG inside a STEM with EELS capabilities. (Top right) Optical image of the same sample with a dotted red outline showing the region where STEM is performed. (Center right) ADF image of the same sample. (Bottom right) EELS of the same sample with labels onmore » the signals for chlorine (green), carbon (blue), and iron (yellow) atoms.« less
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Works referenced in this record:

Generalized Gradient Approximation Made Simple
journal, October 1996

  • Perdew, John P.; Burke, Kieron; Ernzerhof, Matthias
  • Physical Review Letters, Vol. 77, Issue 18, p. 3865-3868
  • DOI: 10.1103/PhysRevLett.77.3865

Nonadiabatic Kohn Anomaly in a Doped Graphene Monolayer
journal, December 2006

Projector augmented-wave method
journal, December 1994

Issues and challenges facing rechargeable lithium batteries
journal, November 2001

  • Tarascon, J.-M.; Armand, M.
  • Nature, Vol. 414, Issue 6861, p. 359-367
  • DOI: 10.1038/35104644

Hybrid functionals based on a screened Coulomb potential
journal, May 2003

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 118, Issue 18
  • DOI: 10.1063/1.1564060

Tuning two-dimensional nanomaterials by intercalation: materials, properties and applications
journal, January 2016

  • Wan, Jiayu; Lacey, Steven D.; Dai, Jiaqi
  • Chemical Society Reviews, Vol. 45, Issue 24
  • DOI: 10.1039/C5CS00758E

Heterointerface effects in the electrointercalation of van der Waals heterostructures
journal, June 2018

Unforeseen high temperature and humidity stability of FeCl3 intercalated few layer graphene
journal, January 2015

  • Wehenkel, Dominique Joseph; Bointon, Thomas Hardisty; Booth, Tim
  • Scientific Reports, Vol. 5, Issue 1
  • DOI: 10.1038/srep07609

FeCl 3 intercalated few-layer graphene for high lithium-ion storage performance
journal, January 2015

  • Qi, Xin; Qu, Jin; Zhang, Hao-Bin
  • Journal of Materials Chemistry A, Vol. 3, Issue 30
  • DOI: 10.1039/C5TA03087K

Approaching Magnetic Ordering in Graphene Materials by FeCl 3 Intercalation
journal, March 2014

  • Bointon, Thomas Hardisty; Khrapach, Ivan; Yakimova, Rositza
  • Nano Letters, Vol. 14, Issue 4
  • DOI: 10.1021/nl4040779

Spiral magnetic structure of Fe in Van der Waals gapped FeOCl and polyaniline-intercalated FeOCl
journal, December 2000

Vacancy-Driven Anisotropic Defect Distribution in the Battery-Cathode Material LiFePO 4
journal, August 2011

From ultrasoft pseudopotentials to the projector augmented-wave method
journal, January 1999

Excitonic Effects on the Optical Response of Graphene and Bilayer Graphene
journal, October 2009

Intercalation of Few-Layer Graphite Flakes with FeCl 3 : Raman Determination of Fermi Level, Layer by Layer Decoupling, and Stability
journal, April 2011

  • Zhao, Weijie; Tan, Ping Heng; Liu, Jian
  • Journal of the American Chemical Society, Vol. 133, Issue 15
  • DOI: 10.1021/ja110939a

Electrical control of 2D magnetism in bilayer CrI3
journal, April 2018

Theory-assisted determination of nano-rippling and impurities in atomic resolution images of angle-mismatched bilayer graphene
journal, September 2018

  • Ovchinnikov, Oleg S.; O’Hara, Andrew; Nicholl, Ryan J. T.
  • 2D Materials, Vol. 5, Issue 4
  • DOI: 10.1088/2053-1583/aadb5f

The structures of some ferric chloride–graphite compounds
journal, May 1956

Erratum: “Hybrid functionals based on a screened Coulomb potential” [J. Chem. Phys. 118, 8207 (2003)]
journal, June 2006

  • Heyd, Jochen; Scuseria, Gustavo E.; Ernzerhof, Matthias
  • The Journal of Chemical Physics, Vol. 124, Issue 21
  • DOI: 10.1063/1.2204597

Two-dimensional heterostructures for energy storage
journal, June 2017

Li-ion battery materials: present and future
journal, June 2015

Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping
journal, April 2014

Discovery of Intrinsic Ferromagnetism in Two-Dimensional van der Waals Crystals
conference, January 2017

  • Gong, Cheng; Li, Lin; Li, Zhenglu
  • CLEO: Applications and Technology, Conference on Lasers and Electro-Optics
  • DOI: 10.1364/cleo_at.2017.jth5c.2

Reversible superdense ordering of lithium between two graphene sheets
journal, November 2018

Chiral tunnelling and the Klein paradox in graphene
journal, August 2006

  • Katsnelson, M. I.; Novoselov, K. S.; Geim, A. K.
  • Nature Physics, Vol. 2, Issue 9
  • DOI: 10.1038/nphys384

Refinement of the crystal structure of iron oxychloride
journal, August 1970

  • Lind, M. D.
  • Acta Crystallographica Section B Structural Crystallography and Crystal Chemistry, Vol. 26, Issue 8
  • DOI: 10.1107/S0567740870003618

Ligand-field helical luminescence in a 2D ferromagnetic insulator
journal, December 2017

Synthesis and Electrical Characterization of Magnetic Bilayer Graphene Intercalate
journal, February 2011

  • Kim, Namdong; Kim, Kwang S.; Jung, Naeyoung
  • Nano Letters, Vol. 11, Issue 2
  • DOI: 10.1021/nl104228f

Discovery of intrinsic ferromagnetism in two-dimensional van der Waals crystals
journal, April 2017

Feature extraction via similarity search: application to atom finding and denoising in electron and scanning probe microscopy imaging
journal, March 2018

  • Somnath, Suhas; Smith, Christopher R.; Kalinin, Sergei V.
  • Advanced Structural and Chemical Imaging, Vol. 4, Issue 1
  • DOI: 10.1186/s40679-018-0052-y

Electric-field switching of two-dimensional van der Waals magnets
journal, March 2018

Novel Highly Conductive and Transparent Graphene-Based Conductors
journal, April 2012

  • Khrapach, Ivan; Withers, Freddie; Bointon, Thomas H.
  • Advanced Materials, Vol. 24, Issue 21
  • DOI: 10.1002/adma.201200489

Electronic structure of AlFeN films exhibiting crystallographic orientation change from c- to a-axis with Fe concentrations and annealing effect
journal, February 2020

Intercalation compounds of graphite
journal, January 2002

Chiral superconductivity from repulsive interactions in doped graphene
journal, January 2012

  • Nandkishore, Rahul; Levitov, L. S.; Chubukov, A. V.
  • Nature Physics, Vol. 8, Issue 2
  • DOI: 10.1038/nphys2208

Li intercalation at graphene/hexagonal boron nitride interfaces
journal, June 2016

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

Challenges in the development of advanced Li-ion batteries: a review
journal, January 2011

  • Etacheri, Vinodkumar; Marom, Rotem; Elazari, Ran
  • Energy & Environmental Science, Vol. 4, Issue 9
  • DOI: 10.1039/c1ee01598b

Quantum interference and Klein tunnelling in graphene heterojunctions
journal, February 2009

  • Young, Andrea F.; Kim, Philip
  • Nature Physics, Vol. 5, Issue 3
  • DOI: 10.1038/nphys1198

Layer-dependent ferromagnetism in a van der Waals crystal down to the monolayer limit
journal, June 2017

  • Huang, Bevin; Clark, Genevieve; Navarro-Moratalla, Efrén
  • Nature, Vol. 546, Issue 7657
  • DOI: 10.1038/nature22391

Semiempirical GGA-type density functional constructed with a long-range dispersion correction
journal, January 2006

  • Grimme, Stefan
  • Journal of Computational Chemistry, Vol. 27, Issue 15, p. 1787-1799
  • DOI: 10.1002/jcc.20495

Reducing Dzyaloshinskii-Moriya interaction and field-free spin-orbit torque switching in synthetic antiferromagnets
journal, May 2021

Model for superconductivity in graphite intercalation compounds
journal, July 1983

An electron microscope for the aberration-corrected era
journal, February 2008

Superconductivity in the intercalated graphite compounds C6Yb and C6Ca
journal, September 2005

  • Weller, Thomas E.; Ellerby, Mark; Saxena, Siddharth S.
  • Nature Physics, Vol. 1, Issue 1
  • DOI: 10.1038/nphys0010

Controlling inelastic light scattering quantum pathways in graphene
journal, March 2011

  • Chen, Chi-Fan; Park, Cheol-Hwan; Boudouris, Bryan W.
  • Nature, Vol. 471, Issue 7340
  • DOI: 10.1038/nature09866

Intercalation compounds of graphite
journal, April 1981

Intercalation of few-layer graphite flakes with FeCl3: Raman determination of Fermi level, layer by layer decoupling, and stability.
text, January 2011

  • Zhao, Weijie; Tan, Ping Heng; Liu, Jian
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.33436

Deterministic transfer of two-dimensional materials by all-dry viscoelastic stamping
preprint, January 2013

Approaching magnetic ordering in graphene materials by FeCl$_3$ intercalation
text, January 2015

Layer-dependent Ferromagnetism in a van der Waals Crystal down to the Monolayer Limit
text, January 2017

Electrical Control of 2D Magnetism in Bilayer CrI3
text, January 2018

Electric-field switching of two-dimensional van der Waals magnets
text, January 2018

Chiral tunneling and the Klein paradox in graphene
text, January 2006

Non-adiabatic Kohn-anomaly in a doped graphene monolayer
text, January 2006

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    Figures / Tables found in this record:

    FIG. 1 (p. 3)figure
    FIG. 2 (p. 4)figure
    FIG. 3 (p. 5)figure
    FIG. 4 (p. 6)figure
    FIG. 5 (p. 8)figure
    FIG. 6 (p. 9)figure
    FIG. S1 (p. 16)figure
    FIG. S2 (p. 17)figure
    Table S1 (p. 17)table
    FIG. S3 (p. 18)figure
    FIG. S4 (p. 19)figure
    FIG. S5 (p. 22)figure
    FIG. S6 (p. 23)figure
    FIG. S7 (p. 25)figure
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