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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. doi:10.1039/C9NR03504D.
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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
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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.
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@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 = {Tue Jul 23 00:00:00 EDT 2019},
month = {Tue Jul 23 00:00:00 EDT 2019}
}
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Journal Article:
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Publisher's Version of Record
https://doi.org/10.1039/C9NR03504D
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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
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