  Graphene-based nanofolds (GNFs) are edge-connected 2D stacked monolayers
originated from single-layer graphene. Graphene-based nanoscrolls (GNSs) are
nanomaterials with geometry resembling graphene layers rolled up into a spiral
(papyrus-like) form. Both GNSs and GNFs structures induce significant changes
in the mechanical and optoelectronic properties of single-layer graphene,
aggregating new functionalities in carbon-based applications. Here, we carried
our fully atomistic reactive (ReaxFF) molecular dynamics simulations to study
the competition between self-folding and self-scrolling of a graphene sheet. We
adopted initial edge-scrolled graphene (ESG($\phi$,$\theta$)) structures with
similar (or different) twist angles ($\phi$,$\theta$) in each edge, mimicking
the initial configuration that was experimentally developed to form biscrolled
sheets. Results showed that ESG(0,$2\pi$) and ESG(2$\pi$,$2\pi$) evolved to
single-folded and two-folded fully stacked morphologies, respectively. As a
general trend, for twist angles higher than $2\pi$, the self-deformation
process of ESG morphologies yields GNSs. Edge twist angles lower than $\pi$ are
not enough for triggering the self-deformation processes. In the ESG(0,3$\pi$)
and ESG(3$\pi$,3$\pi$) cases, after a relaxation period, their morphology
transition towards GNS occurred rapidly. In the ESG(3$\pi$,3$\pi$) dynamics, a
metastable biscroll was formed by the competition between the left- and
right-sided partial scrolling in forming a unique GNS. At high-temperature
perturbations, the edge folding and scrolling transitions to GNFs and GNSs
occurred within the ultrafast period. Remarkably, the ESG(2$\pi$,3$\pi$)
evolved to a dual state that combines folded and scrolled structures in a
temperature-independent process.
