This thesis demonstrates that layered heterostructures of
two-dimensional crystals graphene, hexagonal boron nitride, and
transition metal dichalcogenides provide new and interesting
interlayer transport phenomena. Low-energy electron microscopy is
employed to study the surface of atomically thin WSe2 prepared by
metal-organic chemical vapor deposition on epitaxial graphene
substrates, and a method for unambiguously measuring the number of
atomic layers is presented. Using very low-energy electrons to
probe the surface of similar heterostructures, a relationship
between extracted work function differences from the layers and the
nature of the electrical contact between them is revealed. An
extension of this analysis is applied to surface studies of MoSe2
prepared by molecular beam epitaxy on epitaxial graphene. A large
work function difference is measured between the MoSe2 and
graphene, and a model is provided which suggests that this
observation results from an exceptional defect density in the MoSe2
film. The thesis expounds a theory for computing tunneling currents
between two-dimensional crystals separated by a thin insulating
barrier; a few situations resulting in resonant tunneling and
negative differential resistance are illustrated by computed
examples, as well as observed characteristics, for monolayer and
bilayer graphene tunneling junctions and transistors.
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