  Atomically thin graphene exhibits fascinating mechanical properties, although
its hardness and transverse stiffness are inferior to those of diamond. To
date, there hasn't been any practical demonstration of the transformation of
multi-layer graphene into diamond-like ultra-hard structures. Here we show that
at room temperature and after nano-indentation, two-layer graphene on SiC(0001)
exhibits a transverse stiffness and hardness comparable to diamond, resisting
to perforation with a diamond indenter, and showing a reversible drop in
electrical conductivity upon indentation. Density functional theory
calculations suggest that upon compression, the two-layer graphene film
transforms into a diamond-like film, producing both elastic deformations and
sp2-to-sp3 chemical changes. Experiments and calculations show that this
reversible phase change is not observed for a single buffer layer on SiC or
graphene films thicker than 3 to 5 layers. Indeed, calculations show that
whereas in two-layer graphene layer-stacking configuration controls the
conformation of the diamond-like film, in a multilayer film it hinders the
phase transformation.
