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Outstanding Properties of Epitaxial Graphene Grown from Silicon Carbide Substrate by Amira Ben Gouider Trabelsi Thesis Submitt

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Outstanding Properties of Epitaxial Graphene Grown from Silicon Carbide Substrate by Amira Ben Gouider Trabelsi Thesis Submitt Outstanding properties of epitaxial graphene grown from silicon carbide substrate by Amira Ben Gouider Trabelsi Thesis Submitted in partial fulfillment of the requirements for the award of Doctor of Philosophy of Loughborough University © by Amira Ben Gouider Trabelsi (2018) 2 5 To my Mother 6 Title: Outstanding properties of epitaxial graphene grown from silicon carbide substrate Abstract In this thesis a study of outstanding properties of epitaxial graphene on SiC were carried out involving Raman spectroscopy, AFM, UFM, XPS, Photoelectric effect and electrical resistivity. Epitaxial graphene was grown from a semi-insulating on-axis 6H (000-1) or 4H-SiC (000-1) substrate. Epitaxial growth is based on Si atoms sublimation from the SiC substrate bulk. We used the basics of epitaxial graphene growth; however small details were changed. This allowed the growth of various layers, new features and new properties. X-ray photoelectron spectroscopy ‘‘XPS’’ was used to identify the different components forming within the graphene – substrate system. The graphene layer number is evidenced by XPS. Atoms percentages in the grown graphene layer were determined. Furthermore, the oxidation of the graphene layers was clearly distinguished. Atomic force microscopy “AFM” was carried out to study the topography response of the graphene sample. This distinguishes any morphological changes of the graphene layer. The size, orientation and regularity of the layers terraces were determined. For the first time, new features such as: island, bubbles and domes of graphene layers were identified. The nature of these features was determined using ultra force microscopy “UFM”. High-resolution micro-Raman (Jobin Yvon HR LabRAM) was employed to illustrate all the revealed properties. Nonetheless, it illustrates the doping, defects, disorder, number of layers and phonon-plasmon coupling of epitaxial graphene. These properties were carefully demonstrated based on local Raman mapping. The findings of these investigations indicate the formation of various types of epitaxial graphene layers. These latest could have various forms with new electrical properties. This was illustrated using a comparative study to mechanical properties of epitaxial graphene island. In fact, new charge distribution was found across these features. These findings also differs from other electrical properties found in flat graphene layers. These latest shows 7 electroneutrality of charge distribution between graphene – SiC substrate. Here, Phonons- plasmons coupling in epitaxial graphene – SiC substrate system were illustrated. On other hand, epitaxial graphene properties were not limited to the graphene layers flatness. In fact, new photoresponse of epitaxial graphene under violet light was revealed. Here, photo resistance increase during to epitaxial graphene morphology. 8 Acknowledgements I wish to thank my supervisor Professor. Feodor V Kusmartsev for his excellent guidance during the course of the project and his precious help through all the stages of my research, his support has by far exceeded my expectations. I would also like to thank Dr Marat Gaifullin for supporting me and provided me with advice to succeed and fulfil my research. Also, I would thank him for the long hours of help in Lab. I extend my thanks to Dr Olga Kusmartseva for her tremendous help and advice, without her continuous effort my research could not have been conducted. I am particularly grateful to Dr Anna Kusmarseva for her valued assistance. Thanks to be address to Mikael Forester for his support during my PhD and collaboration. Also, thanks for Brian Dennis and Phil Sutton for the technical assistance and support with the Lab. Many thanks to my mother, my father, my sister and brother for their love and support which stays an eternal debt for me. Not to forget my friends Dr Samir El Khawaja and his Familly, Dr Nebil and his family, Amjaad and her Mum, Hana, Sara and Ann in Loughborough for their encouragement and help. 9 Introduction……………………………………………………………………………..14 Chapter 1: Epitaxial graphene properties………………………………….…18 I- Introduction ……………………………………………………………………………19 II- Fundamental properties of graphene …………………………...……………..20 II-1- Crystal structure…………………………………….………………………...20 II-2- Electronic Structure…………………………………………..……………….21 Exceptional behaviour at the vicinity of K and K'………….………23 Half-integer quantum Hall effect………………………………….....26 II-3- Mechanical properties of graphene…………………………………………..27 II-4- Vibrational properties …………………………………….......………...….27 II-5- Photoeffect…………………………………………………………………...…28 III- Epitaxial graphene…………………………………………………………..…….29 III-1- Silicon carbide (SiC) substrate………………..……………………………..29 III-1-1- SiC structural properties ………………………………………….30 III-1-2-Applications…………………………………..……………………..31 III-2- Graphitization from SiC……………………………………………..………32 III-2-1 Graphene on SiC face terminated Si………………………...……..32 Structural properties ………………………………………....32 6R3-SiC phase properties……………………………………..33 Epitaxial growth of carbon layers……………………………34 Electronic structure…………………………...………………34 Transport properties…………………………….……………35 III-2-2- Graphene on SiC face terminated C: SiC ……………….36 Structural properties………………………………………….36 Electronic properties………………………………………….36 Transport properties of the system……………..……………37 IV- Applications…………………………………………………………………….…….37 V- conclusion…………………………………………………...…………………………38 References :..........................................................................................................................39 Chapter II: Characterization technique……………………………………….…..43 I- Introduction………………………………………………….........................................44 10 II- Graphene surface analysis………………………………………...……………….44 1 optical microscopy……………………………………...………………………44 2- Atomic Force Microscopy (AFM)…………………………….………………45 II-2- 1 Principle of the AFM……………………………..………………….45 3- Ultrasonic force microscopy (UFM)………………………………………….47 II-3-1- Principle of the UFM………………………………………...………47 4- Raman Spectroscopy…………………………………………………….…….48 II-4-1- Principal………………………………………………...……………48 Classical description of the Raman phenomenon…………………..…………………………….……………49 The quantum mechanical description of the Raman .......................………………..………………….49 a- First order Raman effect……………………………………...51 b- Second order Raman effect……………………………………53 c- Raman polarization effect…………….………………………..53 d- Experimental set up…………………….………….……………..54 II-5- Photoelectric effect………………………………………………………………56 II-5-1- Principal………………………………………….……………….56 II-5-2- Experimental set up………………………………...……………….57 III- Conclusion……………………………………………………………………………57 References:…………………………………………………………………………….…..58 Chapter 3: Graphene Localisation: Mechanical and electrical properties variation …………………………………..……………………………………………….60 I- Introduction……………………………………..……….……………………………..61 II- Raman spectra..............................................................................................................61 1- Silicon Carbide…………………………………………………………................61 SiC polytypes ................................................................................61 Raman Spectrum of SiC...............................................................61 2- Graphene Raman spectra……………………….………………..………………62 III- Mechanical properties investigation..................................................................64 1- Epitaxial graphene macro-island...........................................................................64 2- Strain distribution analysis……………………………………………….………66 11 3- Strain effect………………………………………………………………..………67 3-1- Temperature effect on a formation of strain in epitaxial graphene ………………………………………………………….………….…..69 3-2- Estimation of the strain effect on graphene modes………….…..………..70 IV- Electrical properties.................................................................................................75 1- Surface morphology: epitaxial graphene nano-domes and macro- bubbles………………………………………………………………………....75 AFM measurements....................................................................75 UFM measurements………………………………….……..….77 V- EGS properties…………………………………………………………….…..........79 1- Raman mapping Localisation of EGS...................................................................79 2- Capacitor effect on epitaxial graphene bubble….............................…….……..82 3- Charge distribution in epitaxial graphene bubbles.............................................82 4- Quantum capacitance…………….........................................................................84 VI- Conclusion…….............................................................................................……..…87 References………............................................................................................……....88 Chapter 4 : Phonons plasmons coupling…………………….…………….………92 I- Introduction…………………………………………………………………………....93 II- Plasma in the solid state: characteristic and property……………….….93 1- Low coupling…………………………………………………………..………….93 1-1 Screening Length.............................................................................................95 1-2 Plasma Frequency………………………………….…………………95 1-3 Dielectric Function…………………………………..………………..96 III- Inelastic scattering and plasmons…………………….…………………..97 1- Diffusion of light by electron plasmas in semiconductors…………………...…98 1-1 Dynamic structure factor………………………………...……………..99 1-2 Phonon-plasmon coupling……………………………………..……….99 IV- Study of the substrate-graphene interface………………………………101
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