Electronic structure of single and few layered graphene studied by angle resolved photoemission spectro-microscopy.

This thesis reports the study of electronic band structure of single and few layered graphene grown by thermal decomposition of SiC at the surface and by C-sublimation on Ru single crystals. Growth conditions were optimized in order to obtain big few micrometer sized graphene domains. For the first system twisted multilayer graphene domains were found and chosen for study. On ruthenium only single layer graphene domains and also the domains with incorporated bilayer patches were obtained and their electronic properties were investigated after oxidation-reduction reactions at graphene/Ru interface. The electronic band structure was analyzed using high resolution angle resolved photoelectron spectroscopy. In order to obtain spectra from individual domains novel spectromicroscopy end station was used for focusing synchrotron radiation beam to sub-micrometer spot on the sample surface. Experimental results on twisted graphene confirmed interlayer coupling and resulting van Hove singularities, graphene Dirac fermions velocity renormalization and other exotic phenomena predicted by theoretical calculations and partially observed by scanning tunneling spectroscopy technique. Particular attention has been paid to poorly studied interlayer coupling in trilayer systems where middle layer has two different couplings being sandwiched between differently twisted layers. These multilayer graphene domains were also investigated in detail upon alkali metal intercalation and unexpected splitting of upper part of Dirac cone, related to graphene sublattice symmetry breaking in the middle graphene layer was found. In graphene on Ru it was first confirmed that oxidation of Ru under graphene decouples its strongly hybridized π orbitals making graphene p-doped. Our observations indicate that bilayer patches incorporated into single layer background remain n-doped and decorated by intercalated oxygen, thereby forming lateral p-n junctions in the same graphene layer. It was found that hydrogen atmosphere helps to reduce RuOx without the formation of carbon vacancy defects. However, structural wrinkle patterns appeared due to loss of original graphene/Ru epitaxial order remain, and in big graphene domains they can trap H2+RuOx reaction products, making graphene fully decoupled and undoped.