Preparation and Characterization of Van der Waals Heterostructures

In this dissertation different van der Waals heterostructures such as graphene-MoS2 and MoTe2-MoS2 were prepared and characterized. In the first heterostructure, polycrystalline graphene was synthesized by chemical vapor deposition and transferred on top of MoS2 single crystal. In the second heterostructure, MoTe2 monolayers were deposited on MoS2 by molecular beam epitaxy. Characterization of graphene-MoS2 heterostructures was conducted by spin and angle resolve spectroscopy which showed that the electronic structure of the bulk MoS2 and graphene in this van der Waals heterostructures is modified. For MoS2 underneath the graphene, a band structure renormalization and spin polarization are observed. The band structure of MoS2 is modified because the graphene induces screening which shifts the Г-point ~150 meV to lower binding compared to the sample without graphene. The spin polarization is explained by the dipole arising from band bending which breaks the symmetry at the MoS2 surface. For graphene, the band structure at lower binding energy shows that the Dirac cone remains intact with no significant doping. Instead, away from the Fermi level the formation of several gaps in the pi-band due to hybridization with states from the MoS2 is observed. For the heterostructures made depositing monolayer of MoTe2 on MoS2, the morphology, structure and electronic structure were studied. Two dimensional growth is observed under tellurium rich growth conditions and a substrate temperature of 200 °C but formation of a complete monolayer was not achieved. The obtained MoTe2 monolayer shows a high density of the mirror-twins grain boundaries arranged in a pseudo periodic wagon wheel pattern with a periodicity of ~2.6 nm. These grain boundary are formed due to Te-deficiency during the growth. The defect states from these domain boundary pin the Fermi level in MoTe2 and thus determine the band alignment in the MoTe2-MoS2 heterostructures