A study of the nucleation and growth mechanism of graphene on copper
Author(s)
Kim, HoKwon
Type
Thesis
Abstract
Two approaches for the large scale synthesis of graphene were investigated with the objective
of achieving high-quality graphene for practical applications: (1) non-covalent solution based
exfoliation of graphite, and (2) chemical vapour deposition of graphene on copper. As the
processing conditions, structure, and properties of graphene are inherently connected, the aim
of the study was to gain fundamental insights on the critical mechanisms that govern the
properties and device performance of graphene. The first part of this thesis describes the
efficient non-covalent exfoliation of graphite to produce few-layer-graphene dispersion in N-methylpyrrolidone
and large-scale thin film deposition using the Langmuir-Blodgett
assembly. In the second part, the chemical vapour deposition of polycrystalline graphene
films on copper was investigated as it has emerged as the most promising route toward large
scale synthesis of monolayer graphene for optoelectronics applications due to its properties
approaching that of ideal graphene and the relatively low cost of copper. An extensive range
of growth parameters was employed to develop a model of two-dimensional nucleation and
self-limited growth of graphene on the surface of copper. The analysis of the nucleation and
growth kinetics has revealed the relationship between atomic processes that impart two
distinct temperature regimes of nucleation, whereas the growth of the individual nuclei was
shown to be rate-limited by the carbon attachment at the nuclei edges. Moreover, the growth
on high index copper surfaces has shown that graphene nanostructures of controlled shapes,
density, and dimensions can be produced, depending on the Cu crystal orientation.
Interestingly, few-layer-graphene grown on Cu frequently exhibits AA stacking with
interlayer spacing of ~3.6 Å , with a preserved linear dispersion relationship. This work thus
provides practical guidelines for achieving wafer scale single crystal graphene as well as the
control over the mesoscale structure by the careful selection of the growth parameters.
of achieving high-quality graphene for practical applications: (1) non-covalent solution based
exfoliation of graphite, and (2) chemical vapour deposition of graphene on copper. As the
processing conditions, structure, and properties of graphene are inherently connected, the aim
of the study was to gain fundamental insights on the critical mechanisms that govern the
properties and device performance of graphene. The first part of this thesis describes the
efficient non-covalent exfoliation of graphite to produce few-layer-graphene dispersion in N-methylpyrrolidone
and large-scale thin film deposition using the Langmuir-Blodgett
assembly. In the second part, the chemical vapour deposition of polycrystalline graphene
films on copper was investigated as it has emerged as the most promising route toward large
scale synthesis of monolayer graphene for optoelectronics applications due to its properties
approaching that of ideal graphene and the relatively low cost of copper. An extensive range
of growth parameters was employed to develop a model of two-dimensional nucleation and
self-limited growth of graphene on the surface of copper. The analysis of the nucleation and
growth kinetics has revealed the relationship between atomic processes that impart two
distinct temperature regimes of nucleation, whereas the growth of the individual nuclei was
shown to be rate-limited by the carbon attachment at the nuclei edges. Moreover, the growth
on high index copper surfaces has shown that graphene nanostructures of controlled shapes,
density, and dimensions can be produced, depending on the Cu crystal orientation.
Interestingly, few-layer-graphene grown on Cu frequently exhibits AA stacking with
interlayer spacing of ~3.6 Å , with a preserved linear dispersion relationship. This work thus
provides practical guidelines for achieving wafer scale single crystal graphene as well as the
control over the mesoscale structure by the careful selection of the growth parameters.
Date Issued
2012-11
Date Awarded
2013-03
Copyright Statement
Attribution NoDerivatives 4.0 International Licence (CC BY-ND)
Advisor
Saiz Gutierrez, Eduardo
Mattevi, Cecilia
Sponsor
Imperial College London ; Leverhulme Trust ; Engineering and Physical Sciences Research Council ; Natural Sciences and Engineering Research Council of Canada
Publisher Department
Materials
Publisher Institution
Imperial College London
Qualification Level
Doctoral
Qualification Name
Doctor of Philosophy (PhD)