Graphene, an atomically thin material consisting of a hexagonal, highly packed carbon lattice, is of great interests in its magnetic properties. These interests can be categorized in several fields: graphene-based magnetic materials and their applications, large diamagnetism of graphene, and the heterostructures of graphene and other two dimensional materials. In the first aspect, magnetic moments can be in theory introduced to graphene by minimizing its size or introducing structural defects, leading to a very light magnetic material. Furthermore, weak spin-orbital interaction, and long spin relaxation length make graphene promising for spintronics. The first part of this thesis addressed our experimental investigation in defect-induced magnetism of graphene. Non-interacted spins of graphene have been observed by intentionally introducing vacancies and adatoms through ion-irradiation and fluorination, respectively. The defect concentration or the magnetic moments introduced in this thesis cannot provide enough interaction for magnetic coupling. Furthermore, the spins induced by vacancies and adatoms can be controlled through shifting the Fermi energy of graphene using molecular doping, where the adatoms were alternatively introduced by annealing in the inert environment. The paramagnetic responses in graphene induced by vacancy-type defects can only be diverted to half of its maximum, while those induced by sp3 defects can be almost completely suppressed. This difference is supposed that vacancy-type defects induced two localized states (pie and sigma). Only the latter states, which is also the only states induced by sp3 defects, involves in the suppression of magnetic moments at the maximum doping achieved in this thesis. The observation through high resolution transmission electron microscope (HR-TEM) provides more information to the hypothesis of the previous magnetic findings. Reconstructed single vacancy is the majority of defects discovered in proton-irradiated graphene. This result verifies the defect-induced magnetic findings in our results, as well as the electronic properties of defected graphene in the literatures. On the other hand, the diamagnetic susceptibility of neutral graphene is suggested to be larger than that of graphite, and vanish rapidly as a delta-like function when graphene is doped. In our result, surprisingly, the diamagnetic susceptibility varies little when the Fermi level is less than 0.3 eV, in contrast with the theory. When the Fermi energy is higher than 0.3 eV, susceptibility then reduces significantly as the trend of graphite. The little variation in susceptibility near the Dirac point is probably attributed to the spatial confinement of graphene nanoflakes, which are the composition of graphene laminates. In the end of this thesis, we discuss the magnetic properties in one of the other two dimensional materials, molybdenum disulfide (MoS2). It is a potential material for graphene-based heterostructure applications. The magnetic moments in MoS2 are shown to be induced by either edges or vacancies, which are introduced by sonication or proton-irradiation, respectively, similar to the suggestions by theories. However, no significant ferromagnetic finding has been found in all of our cases.
|Date of Award||1 Aug 2014|
- The University of Manchester
|Supervisor||Irina Grigorieva (Supervisor)|