Single-layer graphene has been widely researched in recent years due to its perceived technological applicability and its scientific importance as a unique model system with relativistic Dirac Fermions. Because of its unique geometric and electronic structure, the properties of graphene can be tuned or manipulated in several ways. This tunability is important for technological applications in its own right, and it also allows us to study the fundamental properties of Dirac Fermions, including unique many-body interactions and the nature of the quasiparticles at half-filling. This thesis is a detailed examination of the electronic and structural properties of graphene, studied with angle-resolved photoemission spectroscopy (ARPES) and other surface science techniques like low-energy electron microscopy and diffraction.

This thesis is organized as follows. Chapter 1 gives an introduction to the electronic and structural properties of single-layer graphene. It provides a brief historical overview of major theoretical and experimental milestones and sets the stage for the important theoretical and experimental questions that this thesis addresses.

Chapters 2 and 3 describe the experimental setup. Chapter 2 discusses the experimental techniques used in this thesis with particular focus on the mechanics of ARPES. Chapter 3 discusses the different graphene growth techniques that were used to create our sample with particular focus on our characterization of epitaxial graphene on SiC(0001).

Chapters 4 and 5 form the meat of this thesis: they provide a thorough discussion of the electronic properties of graphene as studied by ARPES. Chapter 4 describes how various perturbations can result in the manipulation of the bare electronic band structure, including the deposition of atomic or molecular species on top of an epitaxial graphene sheet as well as the interactions between graphene and its substrate. Chapter 5 describes the many-body physics in single-layer graphene. It begins with a discussion of the electron-electron interaction in undoped graphene, demonstrating that these interactions qualitatively differ from ordinary metals and semiconductors and depart from the standard Fermi liquid picture for quasiparticles; it then continues by describing how screening the electron-electron and electron-impurity interactions can impact the electronic properties of graphene. Chapter 5 ends with a discussion of the doping-dependent coupling strength of the electron-phonon interaction.