skip to main content
DOE PAGES title logo U.S. Department of Energy
Office of Scientific and Technical Information

Title: Revealing interfacial disorder at the growth-front of thick many-layer epitaxial graphene on SiC: a complementary neutron and X-ray scattering investigation

Abstract

Epitaxial graphene on SiC provides both an excellent source of high-quality graphene as well as an architecture to support its application. Although single-layer graphene on Si-face SiC has garnered extensive interest, many-layer graphene produced on C-face SiC could be significantly more robust for enabling applications. Little is known, however, about the structural properties related to the growth evolution at the buried interface for thick many-layer graphene. Using complementary X-ray scattering and neutron reflectivity as well as electron microscopy, we demonstrate that thick many-layer epitaxial graphene exhibits two vastly different length-scales of the buried interface roughness as a consequence of the Si sublimation that produces the graphene. Over long lateral length-scales the roughness is extremely large (hundreds of Å) and it varies proportionally to the number of graphene layers. In contrast, over much shorter lateral length-scales we observe an atomically abrupt interface with SiC terraces. Graphene near the buried interface exhibits a slightly expanded interlayer spacing (~1%) and fluctuations of this spacing, indicating a tendency for disorder near the growth front. Nevertheless, Dirac cones are observed from the graphene while its domain size routinely reaches micron length-scales, indicating the persistence of high-quality graphene beginning just a short distance away from themore » buried interface. Discovering and reconciling the different length-scales of roughness by reflectivity was complicated by strong diffuse scattering and we provide a detailed discussion of how these difficulties were resolved. The insight from this analysis will be useful for other highly rough interfaces among broad classes of thin-film materials.« less

Authors:
 [1];  [2];  [1];  [1]; ORCiD logo [3];  [2]; ORCiD logo [1];  [1];  [1];  [2]; ORCiD logo [1]
+ Show Author Affiliations
  1. Univ. of Missouri, Columbia, MO (United States)
  2. Georgia Inst. of Technology, Atlanta, GA (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Spallation Neutron Source (SNS)
Publication Date:
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:
1546505
Alternate Identifier(s):
OSTI ID: 1544448
Grant/Contract Number:  
AC05-00OR22725
Resource Type:
Accepted Manuscript
Journal Name:
Nanoscale
Additional Journal Information:
Journal Volume: 11; Journal Issue: 30; Journal ID: ISSN 2040-3364
Publisher:
Royal Society of Chemistry
Country of Publication:
United States
Language:
English
Subject:
72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS

Citation Formats

Mazza, A. R., Miettinen, A., Daykin, A. A., He, X., Charlton, T. R., Conrad, M., Guha, S., Lu, Q., Bian, G., Conrad, E. H., and Miceli, P. F.. Revealing interfacial disorder at the growth-front of thick many-layer epitaxial graphene on SiC: a complementary neutron and X-ray scattering investigation. United States: N. p., 2019. Web. https://doi.org/10.1039/C9NR03504D.
Copy to clipboard
Mazza, A. R., Miettinen, A., Daykin, A. A., He, X., Charlton, T. R., Conrad, M., Guha, S., Lu, Q., Bian, G., Conrad, E. H., & Miceli, P. F.. Revealing interfacial disorder at the growth-front of thick many-layer epitaxial graphene on SiC: a complementary neutron and X-ray scattering investigation. United States. https://doi.org/10.1039/C9NR03504D
Copy to clipboard
Mazza, A. R., Miettinen, A., Daykin, A. A., He, X., Charlton, T. R., Conrad, M., Guha, S., Lu, Q., Bian, G., Conrad, E. H., and Miceli, P. F.. Tue . "Revealing interfacial disorder at the growth-front of thick many-layer epitaxial graphene on SiC: a complementary neutron and X-ray scattering investigation". United States. https://doi.org/10.1039/C9NR03504D. https://www.osti.gov/servlets/purl/1546505.
Copy to clipboard
@article{osti_1546505,
title = {Revealing interfacial disorder at the growth-front of thick many-layer epitaxial graphene on SiC: a complementary neutron and X-ray scattering investigation},
author = {Mazza, A. R. and Miettinen, A. and Daykin, A. A. and He, X. and Charlton, T. R. and Conrad, M. and Guha, S. and Lu, Q. and Bian, G. and Conrad, E. H. and Miceli, P. F.},
abstractNote = {Epitaxial graphene on SiC provides both an excellent source of high-quality graphene as well as an architecture to support its application. Although single-layer graphene on Si-face SiC has garnered extensive interest, many-layer graphene produced on C-face SiC could be significantly more robust for enabling applications. Little is known, however, about the structural properties related to the growth evolution at the buried interface for thick many-layer graphene. Using complementary X-ray scattering and neutron reflectivity as well as electron microscopy, we demonstrate that thick many-layer epitaxial graphene exhibits two vastly different length-scales of the buried interface roughness as a consequence of the Si sublimation that produces the graphene. Over long lateral length-scales the roughness is extremely large (hundreds of Å) and it varies proportionally to the number of graphene layers. In contrast, over much shorter lateral length-scales we observe an atomically abrupt interface with SiC terraces. Graphene near the buried interface exhibits a slightly expanded interlayer spacing (~1%) and fluctuations of this spacing, indicating a tendency for disorder near the growth front. Nevertheless, Dirac cones are observed from the graphene while its domain size routinely reaches micron length-scales, indicating the persistence of high-quality graphene beginning just a short distance away from the buried interface. Discovering and reconciling the different length-scales of roughness by reflectivity was complicated by strong diffuse scattering and we provide a detailed discussion of how these difficulties were resolved. The insight from this analysis will be useful for other highly rough interfaces among broad classes of thin-film materials.},
doi = {10.1039/C9NR03504D},
journal = {Nanoscale},
number = 30,
volume = 11,
place = {United States},
year = {2019},
month = {7}
}
Copy to clipboard
Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1039/C9NR03504D
Copyright Statement
Other availability
Search WorldCat Search WorldCat to find libraries that may hold this journal
Citation Metrics:
Cited by: 1 work
Citation information provided by
Web of Science

Figures / Tables:

Fig. 1 Fig. 1: Transverse scan at qz = 0.057 Å −1 for sample C4CE using X-rays. The solid curves are from a fit to four components: the two Yoneda components are purple and green, the specular is red, the diffuse is blue, and the sum of these (including a linear backgroundmore » term which is not pictured) is shown in black. The inset illustrates the scattering geometry. Here $\vec{k}_i$ , $\vec{k}_f$ are the wavevectors of the incident and reflected beam, respectively, and $\vec{q}$ = $\vec{k}_f$ - $\vec{k}_i$ . The dashed line represents a transverse scan across qz and ω is the rocking angle, where ω = 0 is the specular condition at which point qz = 4π sin[2θ/2]/λ.« less
All figures and tables (15 total)
Save / Share:
Export Metadata
Save to My Library
You must Sign In or Create an Account in order to save documents to your library.

Works referenced in this record:

Electronic Confinement and Coherence in Patterned Epitaxial Graphene
journal, May 2006

Ultrahigh electron mobility in suspended graphene
journal, June 2008

  • Bolotin, K. I.; Sikes, K. J.; Jiang, Z.
  • Solid State Communications, Vol. 146, Issue 9-10, p. 351-355
  • DOI: 10.1016/j.ssc.2008.02.024

Mechanically Strong, Electrically Conductive, and Biocompatible Graphene Paper
journal, July 2008

  • Chen, Haiqun; Müller, Marc B.; Gilmore, Kerry J.
  • Advanced Materials, Vol. 20, Issue 18, p. 3557-3561
  • DOI: 10.1002/adma.200800757

Graphene-based composite materials
journal, July 2006

  • Stankovich, Sasha; Dikin, Dmitriy A.; Dommett, Geoffrey H. B.
  • Nature, Vol. 442, Issue 7100, p. 282-286
  • DOI: 10.1038/nature04969

Graphene Based Electrochemical Sensors and Biosensors: A Review
journal, March 2010

  • Shao, Yuyan; Wang, Jun; Wu, Hong
  • Electroanalysis, Vol. 22, Issue 10, p. 1027-1036
  • DOI: 10.1002/elan.200900571

Graphene spintronics
journal, October 2014

  • Han, Wei; Kawakami, Roland K.; Gmitra, Martin
  • Nature Nanotechnology, Vol. 9, Issue 10
  • DOI: 10.1038/nnano.2014.214

Graphene-based devices for measuring pH
journal, March 2018

Graphene based materials: Past, present and future
journal, October 2011

Graphene plasmonics
journal, November 2012

  • Grigorenko, A. N.; Polini, M.; Novoselov, K. S.
  • Nature Photonics, Vol. 6, Issue 11, p. 749-758
  • DOI: 10.1038/nphoton.2012.262

Solid-state decomposition of silicon carbide for growing ultra-thin heteroepitaxial graphite films
journal, September 2002

  • Charrier, A.; Coati, A.; Argunova, T.
  • Journal of Applied Physics, Vol. 92, Issue 5
  • DOI: 10.1063/1.1498962

Large area and structured epitaxial graphene produced by confinement controlled sublimation of silicon carbide
journal, September 2011

  • de Heer, W. A.; Berger, C.; Ruan, M.
  • Proceedings of the National Academy of Sciences, Vol. 108, Issue 41
  • DOI: 10.1073/pnas.1105113108

Chemically Resolved Interface Structure of Epitaxial Graphene on SiC(0001)
journal, November 2013

Structural consequences of hydrogen intercalation of epitaxial graphene on SiC(0001)
journal, October 2014

  • Emery, Jonathan D.; Wheeler, Virginia D.; Johns, James E.
  • Applied Physics Letters, Vol. 105, Issue 16
  • DOI: 10.1063/1.4899142

Interface structure of epitaxial graphene grown on 4H-SiC(0001)
journal, November 2008

Studies of interfacial layers between 4H-SiC (0001) and graphene
journal, April 2010

Exposure of Epitaxial Graphene on SiC(0001) to Atomic Hydrogen
journal, April 2009

  • Guisinger, Nathan P.; Rutter, Gregory M.; Crain, Jason N.
  • Nano Letters, Vol. 9, Issue 4
  • DOI: 10.1021/nl803331q

Wide Band Gap Semiconductor from a Hidden 2D Incommensurate Graphene Phase
journal, December 2016

Semiconducting Graphene from Highly Ordered Substrate Interactions
journal, September 2015

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

Electronic structure of epitaxial graphene grown on the C-face of SiC and its relation to the structure
journal, December 2012

Structural properties of the multilayer graphene/ 4 H − Si C ( 000 1 ¯ ) system as determined by surface x-ray diffraction
journal, June 2007

Diffuse scattering of hard x rays from rough surfaces
journal, September 1992

X-ray and neutron scattering from rough surfaces
journal, August 1988

Temperature and orientation dependence of kinetic roughening during homoepitaxy: A quantitative x-ray-scattering study of Ag
journal, December 1996

Amorphous interface layer in thin graphite films grown on the carbon face of SiC
journal, September 2011

  • Colby, R.; Bolen, M. L.; Capano, M. A.
  • Applied Physics Letters, Vol. 99, Issue 10
  • DOI: 10.1063/1.3635786

Early stage formation of graphene on the C face of 6H-SiC
journal, December 2008

  • Camara, N.; Rius, G.; Huntzinger, J. -R.
  • Applied Physics Letters, Vol. 93, Issue 26
  • DOI: 10.1063/1.3056655

Diffraction from surfaces with randomly distributed steps
journal, August 1982

Highly ordered graphene for two dimensional electronics
journal, October 2006

  • Hass, J.; Feng, R.; Li, T.
  • Applied Physics Letters, Vol. 89, Issue 14
  • DOI: 10.1063/1.2358299

Graphene spintronics
conference, August 2010

  • Shiraishi, Masashi
  • SPIE NanoScience + Engineering, SPIE Proceedings
  • DOI: 10.1117/12.861584
    [ × clear filter / sort ]

    Figures / Tables found in this record:

    Fig. 1 (p. 3)figure
    Fig. 2 (p. 4)figure
    Fig. 3 (p. 4)figure
    Fig. 4 (p. 5)figure
    Table 1 (p. 5)table
    Fig. 5 (p. 6)figure
    Table 2 (p. 6)table
    Fig. 6 (p. 7)figure
    Fig. 7 (p. 7)figure
    Fig. 8 (p. 8)figure
    Table 3 (p. 8)table
    Fig. 10 (p. 9)figure
    Fig. 9 (p. 9)figure
    Fig. 11 (p. 10)figure
    Fig. 12 (p. 10)figure
      [ × clear filter / sort ]
      Figures/Tables have been extracted from DOE-funded journal article accepted manuscripts.

      Similar Records in DOE PAGES and OSTI.GOV collections: