Vertically stacked two-dimensional
van der Waals (vdW) heterostructures
with specific interlayer angles exhibit peculiar physical properties.
Nowadays, most of the stacked layers are fabricated by mechanical
exfoliation followed by precise transfer and alignment with micrometer
spatial accuracy. This stringent ingredient of sample preparation
limits the productivity of device fabrication and the reproducibility
of device performance. Here, we demonstrate the one-pot chemical vapor
deposition growth of hexagonal boron nitride (hBN)/graphene bilayers
with a high-purity moiré phase. The epitaxial intercalation
of graphene under a hydrogen-terminated hBN template leads to convergent
interlayer angles of less than 0.5°. The near 0° stacking
angle shows almost 2 orders of magnitude higher likelihood of occurrence
compared with angles larger than 0.5°. The bilayers show a substantial
enhancement of carrier mobility compared with monolayer graphene owing
to protection from the top hBN layer. Our work proposes a large-scale
fabrication method of hBN/graphene bilayers with a high uniformity
and controlled interlayer rotation and will promote the production
development for high-quality vdW heterostructures.
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