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Probing and Manipulating Graphene Physics at the Atomic Level

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Probing and Manipulating Graphene Physics at the Atomic Level Probing and manipulating graphene physics at the atomic level. Tesis presentada por Héctor González Herrero Para optar al Grado de Doctor en Ciencias Físicas Director de Tesis Iván Brihuega Álvarez Departamento de física de la Materia Condensada Universidad Autónoma de Madrid Probing and manipulating graphene physics at the atomic level. Resumen....................................................................................................................................... 1 Abstract. ....................................................................................................................................... 3 Chapter 1: Using STM/STS to explore graphene physics at the atomic scale. ................... 5 1.1 Introduction. ..................................................................................................................... 6 1.2 STM theory. ...................................................................................................................... 7 1.3 Operational modes of STM. ............................................................................................ 8 1.3.1 Topography. ............................................................................................................... 8 1.3.2 Spectroscopy. .............................................................................................................. 9 1.3.3 Cu(111) surface state: An example of characterization of 2D states. ................ 10 1.4 Experimental set-up. ...................................................................................................... 15 1.4.1 Preparation Chamber. ............................................................................................ 16 1.4.2 LT-STM chamber. .................................................................................................... 17 1.5 What is graphene? .......................................................................................................... 20 1.6 Graphene morphology with STM. ............................................................................... 24 1.7 Dirac-point mapping: e-h puddles on graphene. ........................................................ 26 1.8 Pseudospin and quasiparticle scattering on graphene. .............................................. 29 1.9 Landau levels on graphene. ........................................................................................... 31 1.10 Graphene on metals. .................................................................................................... 35 1.11 Point defects on graphene ........................................................................................... 39 1.11.1 Carbon vacancies. .................................................................................................. 39 1.11.2 Adatoms. ................................................................................................................. 40 1.11.3 Substitutional species. ........................................................................................... 41 1.12 Van Hove singularities and Fermi velocity renormalization on graphene. ......... 43 1.13 STM lithography on graphene. .................................................................................. 47 1.14 Two summarizing examples. ....................................................................................... 49 1.14.1 Atomic collapse in artificial nuclei on graphene ............................................... 49 1.14.2 Artificial graphene lattices. .................................................................................. 51 References. ............................................................................................................................. 53 Chapter 2: Atomic-scale control of graphene magnetism by using hydrogen atoms. ..... 61 2.1 Introduction. ................................................................................................................... 62 2.2 Sample preparation. ....................................................................................................... 67 2.3 Theoretical methods. ...................................................................................................... 71 2.3.1 Theoretical methodology for H on graphene. ..................................................... 71 2.3.2 Band structure and density of states calculated by DFT. ................................... 73 2.4 A single H atom on Gr/SiC(000-1): Emergence of a local magnetic moment in graphene................................................................................................................................. 75 2.4.1 Topography identification...................................................................................... 75 2.4.2 Spectroscopic signature of the graphene magnetic moment induced by single H atoms: Spin-split state. ................................................................................................. 76 2.4.3 Spatial extension of the H induced graphene polarized state. ........................... 78 2.4.4 Confirming H magnetism by doping. .................................................................. 81 2.5 Influence of the underlying graphene layers. ............................................................. 88 2.6 Hydrogen-Hydrogen interaction. ................................................................................ 91 2.7 Manipulating hydrogen magnetism by STM. ............................................................. 94 2.8 Conclusions. .................................................................................................................. 100 References ............................................................................................................................ 101 Chapter 3: Adsorption mechanism of hydrogen on Gr/SiC(000-1) ................................. 105 3.1 Introduction. ................................................................................................................. 106 3.2 Sample preparation. ..................................................................................................... 107 3.3 Identifying atomic H adsorption site by STM: An STM library for H dimers on graphene............................................................................................................................... 109 3.4 H adsorption at RT. ..................................................................................................... 115 3.5 Lowering the temperature: Statistical study of hydrogen dimers adsorbed at 140K. ............................................................................................................................................... 118 3.6 Understanding H adsorption on graphene. .............................................................. 120 3.7 Conclusions. .................................................................................................................. 126 References ............................................................................................................................ 127 Chapter 4: Graphene tunable transparency to tunnelling electrons as a tool to study the local electronic coupling of graphene with the underlying substrate. ............................ 129 4.1. Graphene on metallic substrates. .............................................................................. 130 4.2. Graphene on Cu(111) .................................................................................................. 133 4.2.1 Gr/Cu(111) growth and characterization. ......................................................... 133 4.2.2 Tunable transparency: Seeing on and through graphene. ............................... 135 4.2.3 Gr/Cu(111) electronic properties measured by STM ....................................... 136 4.3 Gr/Cu(111) coupling described by DFT methods ................................................... 144 4.4 Explanation of graphene transparency ...................................................................... 150 4.5 ARPES measurements on Gr/Cu(111) ...................................................................... 154 4.6 Summary of the electronic properties of Gr/Cu(111) by STM, DFT+vdW and ARPES.................................................................................................................................. 156 4.7 Interaction of point defects with Gr/Cu(111) .......................................................... 157 4.7.1 H atoms on Gr/Cu(111) ....................................................................................... 157 4.5.2 C vacancies on Gr/Cu(111) .................................................................................. 163 4.8 Conclusions ................................................................................................................... 166 References ............................................................................................................................ 167 Conclusiones generales ........................................................................................................... 171 General conclusions. ............................................................................................................... 175 List of publications ................................................................................................................. 179 Resumen. En los últimos 12 años, un campo dentro de la física de la
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