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Atomic structure and dynamics study of defects in graphene by aberration-corrected transmission electron microscope

Graphene has grabbed enormous research attention due to its multiple unique properties. These properties, however, can be strongly influenced by lattice imperfections. Aberration corrected transmission electron microscopy (AC-TEM) is one of the leading methods to image two-dimensional materials at the atomic level. This thesis addresses the issue of structure and dynamics characterization of dislocations and grain boundaries (GBs) in graphene with single atom sensitivity using the state-of-the-art AC-TEM in Department of Materials, University of Oxford. My first goal is to understand the interaction between dislocation and the edge of graphene. When a dislocation is located near an edge, a decrease in the rippling and increase of the in-plane rotation occurs relative to the dislocations in the bulk. The increased in-plane rotation near the edge causes bond rotations at the edge of graphene to reduce the overall strain in the system. Dislocations are highly stable and remain fixed in their position even when located within a few lattice spacings from the graphene edge. With the aid of an in situ heating holder, the high temperature behavior of dislocations is then investigated. Control of temperature enables the differentiation of electron beam induced effects and thermally driven processes. An analysis of the dislocation movement shows both climb and glide processes, including new complex pathways for migration and large nanoscale rapid jumps between fixed positions in the lattice. The improved understanding of the high temperature dislocation movement provides insights into annealing processes in graphene and the behavior of defects with increased heat. The in situ heterogeneous nucleation and growth of graphene are also studied within the AC-TEM. The growth mechanism consists of alternating carbon cluster attachment and indentation filling to maintain a uniform growth front of lowest energy. The highly polycrystalline graphene seed is found to evolve with time into a higher order crystalline structure. The motion of GBs is discontinuous and mediated by both bond rotation and atom evaporation. These results provide insights into the formation of crystalline seed domains that are generated during bottom-up graphene synthesis. Finally, the formation, reconfiguration and annihilation of GB loops are demonstrated. It is shown that the GB loop cannot fully relaxed under electron beam irradiation with its terminal state being isolated dislocations far apart from each other. Line defects composed of several adjacent excess-atom defects can be found during the reconfiguration process. This work gives detailed information about the stability and behavior of large GB loops in two dimensional materials.

Identiferoai:union.ndltd.org:bl.uk/oai:ethos.bl.uk:729971
Date January 2016
CreatorsGong, Chuncheng
ContributorsWarner, Jamie
PublisherUniversity of Oxford
Source SetsEthos UK
Detected LanguageEnglish
TypeElectronic Thesis or Dissertation
Sourcehttps://ora.ox.ac.uk/objects/uuid:53bd9a04-71ad-4da8-b982-cb45a005e791

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