Abstract
In the transition from graphene to graphite, the addition of each individual graphene layer
modifies the electronic structure and produces a different material with unique properties.
Controlled growth of few-layer graphene is therefore of fundamental interest and will provide
access to materials with engineered electronic structure. Here we combine isothermal growth
and etching experiments with in situ scanning electron microscopy to reveal the stacking
sequence and interlayer coupling strength in few-layer graphene. The observed
layer-dependent etching rates reveal the relative strength of the graphene–graphene and
graphene–substrate interaction and the resulting mode of adlayer growth. Scanning tunnelling
microscopy and density functional theory calculations confirm a strong coupling between
graphene edge atoms and platinum. Simulated etching confirms that etching can be viewed
as reversed growth. This work demonstrates that real-time imaging under controlled
atmosphere is a powerful method for designing synthesis protocols for sp2 carbon
nanostructures in between graphene and graphite.
