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Title: Large-Area Growth of Turbostratic Graphene on Ni(111) via Physical Vapor Deposition

Abstract

Single-layer graphene has demonstrated remarkable electronic properties that are strongly influenced by interfacial bonding and break down for the lowest energy configuration of stacked graphene layers (AB Bernal). Multilayer graphene with relative rotations between carbon layers, known as turbostratic graphene, can effectively decouple the electronic states of adjacent layers, preserving properties similar to that of SLG. While the growth of AB Bernal graphene through chemical vapor deposition has been widely reported, we investigate the growth of turbostratic graphene on heteroepitaxial Ni(111) thin films utilizing physical vapor deposition. By varying the carbon deposition temperature between 800 –1100 °C, we report an increase in the graphene quality concomitant with a transition in the size of uniform thickness graphene, ranging from nanocrystallites to thousands of square microns. Combination Raman modes of as-grown graphene within the frequency range of 1650 cm-1 to 2300 cm-1, along with features of the Raman 2D mode, were employed as signatures of turbostratic graphene. Bilayer and multilayer graphene were directly identified from areas that exhibited Raman characteristics of turbostratic graphene using high-resolution TEM imaging. In conclusion, Raman maps of the pertinent modes reveal large regions of turbostratic graphene on Ni(111) thin films at a deposition temperature of 1100 °C.

Authors:
 [1];  [2];  [3];  [3];  [1];  [3]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)
  2. Boston Univ., MA (United States)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States)
Publication Date:
Research Org.:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1259265
Alternate Identifier(s):
OSTI ID: 1335423
Report Number(s):
BNL-112043-2016-JA
Journal ID: ISSN 2045-2322; srep19804
Grant/Contract Number:  
AC02-98CH10886; SC0012704; SC00112704
Resource Type:
Accepted Manuscript
Journal Name:
Scientific Reports
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2045-2322
Publisher:
Nature Publishing Group
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; Electronic properties and materials; Synthesis of graphene

Citation Formats

Garlow, Joseph A., Barrett, Lawrence K., Wu, Lijun, Kisslinger, Kim, Zhu, Yimei, and Pulecio, Javier F. Large-Area Growth of Turbostratic Graphene on Ni(111) via Physical Vapor Deposition. United States: N. p., 2016. Web. doi:10.1038/srep19804.
Garlow, Joseph A., Barrett, Lawrence K., Wu, Lijun, Kisslinger, Kim, Zhu, Yimei, & Pulecio, Javier F. Large-Area Growth of Turbostratic Graphene on Ni(111) via Physical Vapor Deposition. United States. https://doi.org/10.1038/srep19804
Garlow, Joseph A., Barrett, Lawrence K., Wu, Lijun, Kisslinger, Kim, Zhu, Yimei, and Pulecio, Javier F. Fri . "Large-Area Growth of Turbostratic Graphene on Ni(111) via Physical Vapor Deposition". United States. https://doi.org/10.1038/srep19804. https://www.osti.gov/servlets/purl/1259265.
@article{osti_1259265,
title = {Large-Area Growth of Turbostratic Graphene on Ni(111) via Physical Vapor Deposition},
author = {Garlow, Joseph A. and Barrett, Lawrence K. and Wu, Lijun and Kisslinger, Kim and Zhu, Yimei and Pulecio, Javier F.},
abstractNote = {Single-layer graphene has demonstrated remarkable electronic properties that are strongly influenced by interfacial bonding and break down for the lowest energy configuration of stacked graphene layers (AB Bernal). Multilayer graphene with relative rotations between carbon layers, known as turbostratic graphene, can effectively decouple the electronic states of adjacent layers, preserving properties similar to that of SLG. While the growth of AB Bernal graphene through chemical vapor deposition has been widely reported, we investigate the growth of turbostratic graphene on heteroepitaxial Ni(111) thin films utilizing physical vapor deposition. By varying the carbon deposition temperature between 800 –1100 °C, we report an increase in the graphene quality concomitant with a transition in the size of uniform thickness graphene, ranging from nanocrystallites to thousands of square microns. Combination Raman modes of as-grown graphene within the frequency range of 1650 cm-1 to 2300 cm-1, along with features of the Raman 2D mode, were employed as signatures of turbostratic graphene. Bilayer and multilayer graphene were directly identified from areas that exhibited Raman characteristics of turbostratic graphene using high-resolution TEM imaging. In conclusion, Raman maps of the pertinent modes reveal large regions of turbostratic graphene on Ni(111) thin films at a deposition temperature of 1100 °C.},
doi = {10.1038/srep19804},
journal = {Scientific Reports},
number = ,
volume = 6,
place = {United States},
year = {Fri Jan 29 00:00:00 EST 2016},
month = {Fri Jan 29 00:00:00 EST 2016}
}

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Works referenced in this record:

Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils
text, January 2009


Massless Fermions in multilayer graphitic systems with misoriented layers
preprint, January 2007


Current saturation in zero-bandgap, top-gated graphene field-effect transistors
journal, September 2008

  • Meric, Inanc; Han, Melinda Y.; Young, Andrea F.
  • Nature Nanotechnology, Vol. 3, Issue 11
  • DOI: 10.1038/nnano.2008.268

Graphene–nickel interfaces: a review
journal, January 2014


Rotational disorder in few-layer graphene films on 6 H Si C ( 000 1 ) : A scanning tunneling microscopy study
journal, April 2008


Raman Signature of Graphene Superlattices
journal, November 2011

  • Carozo, Victor; Almeida, Clara M.; Ferreira, Erlon H. M.
  • Nano Letters, Vol. 11, Issue 11
  • DOI: 10.1021/nl201370m

Raman spectroscopy and imaging of graphene
journal, October 2008


Graphene and Graphene Oxide: Synthesis, Properties, and Applications
journal, June 2010

  • Zhu, Yanwu; Murali, Shanthi; Cai, Weiwei
  • Advanced Materials, Vol. 22, Issue 35, p. 3906-3924
  • DOI: 10.1002/adma.201001068

Comparison of Graphene Growth on Single-Crystalline and Polycrystalline Ni by Chemical Vapor Deposition
journal, October 2010

  • Zhang, Yi; Gomez, Lewis; Ishikawa, Fumiaki N.
  • The Journal of Physical Chemistry Letters, Vol. 1, Issue 20
  • DOI: 10.1021/jz1011466

Long-Range Ordered Single-Crystal Graphene on High-Quality Heteroepitaxial Ni Thin Films Grown on MgO(111)
journal, January 2011

  • Iwasaki, Takayuki; Park, Hye Jin; Konuma, Mitsuharu
  • Nano Letters, Vol. 11, Issue 1
  • DOI: 10.1021/nl102834q

Second-Order Overtone and Combination Raman Modes of Graphene Layers in the Range of 1690−2150 cm −1
journal, February 2011

  • Cong, Chunxiao; Yu, Ting; Saito, Riichiro
  • ACS Nano, Vol. 5, Issue 3
  • DOI: 10.1021/nn200010m

The shear mode of multilayer graphene
journal, February 2012

  • Tan, P. H.; Han, W. P.; Zhao, W. J.
  • Nature Materials, Vol. 11, Issue 4
  • DOI: 10.1038/nmat3245

Direct graphene growth on Co 3 O 4 (111) by molecular beam epitaxy
journal, January 2012


Raman Spectrum of Graphene and Graphene Layers
journal, October 2006


Approaching ballistic transport in suspended graphene
journal, July 2008

  • Du, Xu; Skachko, Ivan; Barker, Anthony
  • Nature Nanotechnology, Vol. 3, Issue 8, p. 491-495
  • DOI: 10.1038/nnano.2008.199

Large-Area Synthesis of High-Quality and Uniform Graphene Films on Copper Foils
journal, May 2009


Rapid Identification of Stacking Orientation in Isotopically Labeled Chemical-Vapor Grown Bilayer Graphene by Raman Spectroscopy
journal, March 2013

  • Fang, Wenjing; Hsu, Allen L.; Caudillo, Roman
  • Nano Letters, Vol. 13, Issue 4, p. 1541-1548
  • DOI: 10.1021/nl304706j

A review of chemical vapour deposition of graphene on copper
journal, January 2011

  • Mattevi, Cecilia; Kim, Hokwon; Chhowalla, Manish
  • J. Mater. Chem., Vol. 21, Issue 10
  • DOI: 10.1039/C0JM02126A

Low-resistance spin injection into silicon using graphene tunnel barriers
journal, September 2012

  • van 't Erve, O. M. J.; Friedman, A. L.; Cobas, E.
  • Nature Nanotechnology, Vol. 7, Issue 11
  • DOI: 10.1038/nnano.2012.161

Raman spectroscopy in graphene
journal, April 2009


Twisting Bilayer Graphene Superlattices
journal, March 2013

  • Lu, Chun-Chieh; Lin, Yung-Chang; Liu, Zheng
  • ACS Nano, Vol. 7, Issue 3
  • DOI: 10.1021/nn3059828

Large Area, Few-Layer Graphene Films on Arbitrary Substrates by Chemical Vapor Deposition
journal, January 2009

  • Reina, Alfonso; Jia, Xiaoting; Ho, John
  • Nano Letters, Vol. 9, Issue 1
  • DOI: 10.1021/nl801827v

Chemical methods for the production of graphenes
journal, March 2009

  • Park, Sungjin; Ruoff, Rodney S.
  • Nature Nanotechnology, Vol. 4, Issue 4, p. 217-224
  • DOI: 10.1038/nnano.2009.58

Precise and Ultrafast Molecular Sieving Through Graphene Oxide Membranes
journal, February 2014


Substrate-limited electron dynamics in graphene
journal, May 2008


Epitaxial Graphene Growth by Carbon Molecular Beam Epitaxy (CMBE)
journal, August 2010

  • Park, Jeongho; Mitchel, William C.; Grazulis, Lawrence
  • Advanced Materials, Vol. 22, Issue 37
  • DOI: 10.1002/adma.201000756

Platinum surface LEED rings
journal, September 1969


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


Effects of Layer Stacking on the Combination Raman modes in Graphene
text, January 2011


General equation for the determination of the crystallite size La of nanographite by Raman spectroscopy
journal, April 2006

  • Cançado, L. G.; Takai, K.; Enoki, T.
  • Applied Physics Letters, Vol. 88, Issue 16
  • DOI: 10.1063/1.2196057

Growth of graphene from solid carbon sources
journal, November 2010


Why Multilayer Graphene on 4 H SiC ( 000 1 ¯ ) Behaves Like a Single Sheet of Graphene
journal, March 2008


Material contrast in SEM: Fermi energy and work function effects
journal, February 2010


Single-Layer Behavior and Its Breakdown in Twisted Graphene Layers
journal, March 2011


Long-Range Ordered Single-Crystal Graphene on High-Quality Heteroepitaxial Ni Thin Films Grown on MgO(111)
journal, January 2011

  • Iwasaki, Takayuki; Park, Hye Jin; Konuma, Mitsuharu
  • Nano Letters, Vol. 11, Issue 1
  • DOI: 10.1021/nl102834q

Graphitization of α-Silicon Carbide
journal, February 1962


Studying disorder in graphite-based systems by Raman spectroscopy
journal, January 2007

  • Pimenta, M. A.; Dresselhaus, G.; Dresselhaus, M. S.
  • Phys. Chem. Chem. Phys., Vol. 9, Issue 11
  • DOI: 10.1039/b613962k

The rise of graphene
journal, March 2007

  • Geim, A. K.; Novoselov, K. S.
  • Nature Materials, Vol. 6, Issue 3, p. 183-191
  • DOI: 10.1038/nmat1849

Raman spectroscopy as a versatile tool for studying the properties of graphene
journal, April 2013


Towards wafer-size graphene layers by atmospheric pressure graphitization of silicon carbide
journal, February 2009

  • Emtsev, Konstantin V.; Bostwick, Aaron; Horn, Karsten
  • Nature Materials, Vol. 8, Issue 3
  • DOI: 10.1038/nmat2382

Growth of large-area single- and Bi-layer graphene by controlled carbon precipitation on polycrystalline Ni surfaces
journal, June 2009


Imaging layer number and stacking order through formulating Raman fingerprints obtained from hexagonal single crystals of few layer graphene
journal, December 2012


Raman Signature of Graphene Superlattices
journal, November 2011

  • Carozo, Victor; Almeida, Clara M.; Ferreira, Erlon H. M.
  • Nano Letters, Vol. 11, Issue 11
  • DOI: 10.1021/nl201370m

Resonance effects on the Raman spectra of graphene superlattices
journal, August 2013


Current saturation in zero-bandgap, top-gated graphene field-effect transistors
journal, September 2008

  • Meric, Inanc; Han, Melinda Y.; Young, Andrea F.
  • Nature Nanotechnology, Vol. 3, Issue 11
  • DOI: 10.1038/nnano.2008.268

Graphene Bilayer with a Twist: Electronic Structure
journal, December 2007

  • Lopes dos Santos, J. M. B.; Peres, N. M. R.; Castro Neto, A. H.
  • Physical Review Letters, Vol. 99, Issue 25
  • DOI: 10.1103/PhysRevLett.99.256802

Graphene and Graphene Oxide: Synthesis, Properties, and Applications
journal, June 2010

  • Zhu, Yanwu; Murali, Shanthi; Cai, Weiwei
  • Advanced Materials, Vol. 22, Issue 35, p. 3906-3924
  • DOI: 10.1002/adma.201001068

Graphene Nucleation on Transition Metal Surface: Structure Transformation and Role of the Metal Step Edge
journal, April 2011

  • Gao, Junfeng; Yip, Joanne; Zhao, Jijun
  • Journal of the American Chemical Society, Vol. 133, Issue 13, p. 5009-5015
  • DOI: 10.1021/ja110927p

A decade of R2R graphene manufacturing
journal, October 2021


Raman spectroscopy of graphene and carbon nanotubes
journal, June 2011


Resonant Raman spectroscopy of twisted multilayer graphene
journal, November 2014

  • Wu, Jiang-Bin; Zhang, Xin; Ijäs, Mari
  • Nature Communications, Vol. 5, Issue 1
  • DOI: 10.1038/ncomms6309

On the mechanisms of precipitation of graphene on nickel thin films
text, January 2011


Raman spectra of out-of-plane phonons in bilayer graphene
journal, July 2011


Rapid Identification of Stacking Orientation in Isotopically Labeled Chemical-Vapor Grown Bilayer Graphene by Raman Spectroscopy
journal, March 2013

  • Fang, Wenjing; Hsu, Allen L.; Caudillo, Roman
  • Nano Letters, Vol. 13, Issue 4, p. 1541-1548
  • DOI: 10.1021/nl304706j

Chemical methods for the production of graphenes
journal, March 2009

  • Park, Sungjin; Ruoff, Rodney S.
  • Nature Nanotechnology, Vol. 4, Issue 4, p. 217-224
  • DOI: 10.1038/nnano.2009.58

Graphene–nickel interfaces: a review
journal, January 2014


Reduction of Fermi velocity in folded graphene observed by resonance Raman spectroscopy
journal, June 2008


Effects of Layer Stacking on the Combination Raman Modes in Graphene
journal, January 2011

  • Rao, Rahul; Podila, Ramakrishna; Tsuchikawa, Ryuichi
  • ACS Nano, Vol. 5, Issue 3
  • DOI: 10.1021/nn1031017

Charged-impurity scattering in graphene
journal, April 2008

  • Chen, J. -H.; Jang, C.; Adam, S.
  • Nature Physics, Vol. 4, Issue 5
  • DOI: 10.1038/nphys935

Raman spectra of misoriented bilayer graphene
journal, September 2008


Second-Order Overtone and Combination Raman Modes of Graphene Layers in the Range of 1690−2150 cm −1
journal, February 2011

  • Cong, Chunxiao; Yu, Ting; Saito, Riichiro
  • ACS Nano, Vol. 5, Issue 3
  • DOI: 10.1021/nn200010m

The shear mode of multilayer graphene
journal, February 2012

  • Tan, P. H.; Han, W. P.; Zhao, W. J.
  • Nature Materials, Vol. 11, Issue 4
  • DOI: 10.1038/nmat3245

The evolution of electronic structure in few-layer graphene revealed by optical spectroscopy
journal, August 2010

  • Mak, K. F.; Sfeir, M. Y.; Misewich, J. A.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 34
  • DOI: 10.1073/pnas.1004595107

Raman spectroscopy as a versatile tool for studying the properties of graphene
journal, April 2013


Sub-surface nucleation of graphene precursors near a Ni(111) step-edge
journal, January 2012

  • Li, Hai-Bei; Page, Alister J.; Wang, Ying
  • Chemical Communications, Vol. 48, Issue 64
  • DOI: 10.1039/c2cc32995f

Resonant Raman spectroscopy of twisted multilayer graphene.
text, January 2014

  • Wu, Jiang-Bin; Zhang, Xin; Ijäs, Mari
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.26738

Massless fermions in multilayer graphitic systems with misoriented layers: Ab initio calculations and experimental fingerprints
journal, November 2007


Roll-to-roll production of 30-inch graphene films for transparent electrodes
journal, June 2010

  • Bae, Sukang; Kim, Hyeongkeun; Lee, Youngbin
  • Nature Nanotechnology, Vol. 5, Issue 8, p. 574-578
  • DOI: 10.1038/nnano.2010.132

Structure and surface morphology of epitaxial Ni films grown on MgO(111) substrates: growth of high quality single domain films
journal, March 1999


Epitaxial Graphene Growth by Carbon Molecular Beam Epitaxy (CMBE)
journal, August 2010

  • Park, Jeongho; Mitchel, William C.; Grazulis, Lawrence
  • Advanced Materials, Vol. 22, Issue 37
  • DOI: 10.1002/adma.201000756

Characterizing Graphene, Graphite, and Carbon Nanotubes by Raman Spectroscopy
journal, August 2010


Material contrast in SEM: Fermi energy and work function effects
journal, February 2010


Measurement of layer breathing mode vibrations in few-layer graphene
journal, March 2013


Longitudinal unzipping of carbon nanotubes to form graphene nanoribbons
journal, April 2009

  • Kosynkin, Dmitry V.; Higginbotham, Amanda L.; Sinitskii, Alexander
  • Nature, Vol. 458, Issue 7240
  • DOI: 10.1038/nature07872

Growth of graphene from solid carbon sources
journal, November 2010


Raman Spectroscopy Study of Rotated Double-Layer Graphene: Misorientation-Angle Dependence of Electronic Structure
journal, June 2012


The evolution of electronic structure in few-layer graphene revealed by optical spectroscopy
journal, August 2010

  • Mak, K. F.; Sfeir, M. Y.; Misewich, J. A.
  • Proceedings of the National Academy of Sciences, Vol. 107, Issue 34
  • DOI: 10.1073/pnas.1004595107

On the mechanisms of precipitation of graphene on nickel thin films
journal, November 2011


Raman Characterization of ABA- and ABC-Stacked Trilayer Graphene
journal, October 2011

  • Cong, Chunxiao; Yu, Ting; Sato, Kentaro
  • ACS Nano, Vol. 5, Issue 11
  • DOI: 10.1021/nn203472f

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


Electronic structure of turbostratic graphene
journal, April 2010


Direct graphene growth on Co 3 O 4 (111) by molecular beam epitaxy
journal, January 2012


Scanning Electron Microscopy and X-ray Microanalysis
book, January 2003


Raman Spectroscopy in Graphene-Based Systems: Prototypes for Nanoscience and Nanometrology
journal, December 2012


Works referencing / citing this record:

A critical review on the contributions of chemical and physical factors toward the nucleation and growth of large-area graphene
text, January 2018

  • Ani, Mh; Kamarudin, Ma; Ramlan, Ah
  • Apollo - University of Cambridge Repository
  • DOI: 10.17863/cam.20958

Two-Dimensional Hallmark of Highly Interconnected Three-Dimensional Nanoporous Graphene
journal, July 2017


Three-dimensional microporous graphene decorated with lithium
journal, August 2018

  • Iacobucci, Marco; Bernardo, Iolanda Di; Christian, Meganne
  • Nanotechnology, Vol. 29, Issue 40
  • DOI: 10.1088/1361-6528/aad3f5

Functionalized Hybridization of 2D Nanomaterials
journal, September 2019


Large scale epitaxial graphite grown on twin free nickel(111)/spinel substrate
journal, January 2020

  • Lu, Zonghuan; Sun, Xin; Xiang, Yu
  • CrystEngComm, Vol. 22, Issue 1
  • DOI: 10.1039/c9ce01515a

Ultrastiff, Strong, and Highly Thermally Conductive Crystalline Graphitic Films with Mixed Stacking Order
journal, May 2019

  • Wang, Bin; Cunning, Benjamin V.; Kim, Na Yeon
  • Advanced Materials, Vol. 31, Issue 29
  • DOI: 10.1002/adma.201903039

Anti-fouling graphene-based membranes for effective water desalination
journal, February 2018


A critical review on the contributions of chemical and physical factors toward the nucleation and growth of large-area graphene
journal, January 2018


Functionalized Hybridization of 2D Nanomaterials
journal, September 2019


Scalable synthesis of gyroid-inspired freestanding three-dimensional graphene architectures
journal, January 2019

  • Garcia, Adrian E.; Wang, Chen Santillan; Sanderson, Robert N.
  • Nanoscale Advances, Vol. 1, Issue 10
  • DOI: 10.1039/c9na00358d

Identification of turbostratic twisting in germanane
journal, January 2019

  • Trout, Amanda H.; Wang, Yaxian; Esser, Bryan D.
  • Journal of Materials Chemistry C, Vol. 7, Issue 32
  • DOI: 10.1039/c9tc02064k

Graphite to Graphene: Green Synthesis Using Opuntia ficus-indica
journal, January 2019

  • Calderón-Ayala, G.; Cortez-Valadez, M.; Acosta-Elías, M.
  • Journal of Electronic Materials, Vol. 48, Issue 3
  • DOI: 10.1007/s11664-018-06918-5

Growth of graphitic carbon layers around silicon carbide nanowires
journal, August 2019

  • Mishra, Neeraj; Bosi, Matteo; Rossi, Francesca
  • Journal of Applied Physics, Vol. 126, Issue 6
  • DOI: 10.1063/1.5098987

Ultrasonication-induced sp 3 hybridization defects in Langmuir–Schaefer layers of turbostratic graphene
journal, January 2018

  • Rytel, K.; Widelicka, M.; Łukawski, D.
  • Physical Chemistry Chemical Physics, Vol. 20, Issue 18
  • DOI: 10.1039/c8cp01363b

Single-step ambient-air synthesis of graphene from renewable precursors as electrochemical genosensor
journal, January 2017

  • Seo, Dong Han; Pineda, Shafique; Fang, Jinghua
  • Nature Communications, Vol. 8, Issue 1
  • DOI: 10.1038/ncomms14217

Gram-scale bottom-up flash graphene synthesis
journal, January 2020