Understanding the crumpling behavior
of two-dimensional (2D) macromolecular
sheet materials is of fundamental importance in engineering and technological
applications. Among the various properties of these sheets, interfacial
adhesion critically contributes to the formation of crumpled structures.
Here, we present a coarse-grained molecular dynamics (CG-MD) simulation
study to explore the fundamental role of self-adhesion in the crumpling
behaviors of macromolecular sheets having varying masses or sizes.
By evaluating the potential energy evolution, our results show that
the self-adhesion plays a dominant role in the crumpling behavior
of the sheets compared to in-plane and out-of-plane stiffnesses. The
macromolecular sheets with higher adhesion tend to form a self-folding
planar structure at the quasi-equilibrium state of the crumpling and
exhibit a lower packing efficiency as evaluated by the fractal dimension
of the system. Notably, during the crumpling process, both the radius
of gyration R
g and the hydrodynamic radius R
h of the macromolecular sheet can be quantitatively
described by the power-law scaling relationships associated with adhesion.
The evaluation of the shape descriptors indicates that the overall
crumpling behavior of macromolecular sheets can be characterized by
three regimes, i.e., the less bent, intermediate, and highly crumpled
regimes, dominated by edge-bending, self-adhesion, and further compression,
respectively. The internal structural analysis further reveals that
the sheet transforms from the initially ordered state to the disordered
glassy state upon crumpling, which can be facilitated by greater self-adhesion.
Our study provides fundamental insights into the adhesion-dependent
structural behavior of macromolecular sheets under crumpling, which
is essential for establishing the structure-processing-property relationships
for crumpled macromolecular sheets.