Nanocrystalline
carbon films containing preferentially oriented
graphene-based nanocrystals within an amorphous carbon matrix have
attracted significant theoretical and experimental interest due to
their favorable chemical and physical properties. At present, there
are intense efforts to study the grain size and growth orientation
of the graphene-based nanocrystals to achieve a controllable growth
of nanocrystalline carbon films. However, despite the frequent use
of plasma-assisted deposition techniques, the atomistic-scale mechanisms,
including the effects of plasma density and energy on the nucleation
process and growth orientation of the graphene-based nanocrystals,
as well as associated dynamic processes involved in deposition processes,
have not yet been thoroughly studied. In this paper, the plasma-assisted
growth of nanocrystalline carbon thin films with preferentially oriented
nanocrystals was systematically studied by hybrid molecular dynamics–Monte
Carlo simulations using a recently developed force field, the charge-implicit
ReaxFF. By combining the experimental data with the atomistic simulations,
we reveal that plasma ion bombardments, in suitable ranges of energies
and densities, allow the highest nucleation density in the nanocrystalline
carbon films. Theoretically optimum windows of the plasma energy and
density are first presented in the form of crystallization phase diagrams.
Furthermore, to investigate the relationship between the growth orientation
and the plasma ion energy, simulations of graphene irradiated with
Ar ions from different incident angles were also performed. On the
basis of the mechanism of “survival of the fittest”,
we proposed using the critical energy of generating the Stone–Thrower–Wales
defects to design the growth orientation of graphite-like nanocrystals
by controlling the plasma ion energy.