Self-assembled
structures of two-dimensional (2D) materials exhibit
novel physical properties distinct from those of their parent materials.
Herein, the critical role of desulfurization on the self-assembled
structural morphologies of molybdenum disulfide (MoS2)
monolayer sheets is explored using molecular dynamics (MD) simulations.
MD results show that there are differences in the atomic energetics
of MoS2 monolayer sheets with different desulfurization
contents. Both free-standing and substrate-hosted MoS2 monolayer
sheets show diversity in structural morphologies, for example, flat
plane structures, wrinkles, nanotubes, and folds, depending on the
desulfurization contents, planar dimensions, and ratios of length
to width of MoS2 sheets. Particularly, at the critical
desulfurization content, they can roll up into nanotubes, which is
in good agreement with previous experimental observations. Importantly,
these observed differences in the molecular structural morphologies
between free-standing and substrate-hosted MoS2 monolayer
sheets can be attributed to interatomic interactions and interlayer
van der Waals interactions. Furthermore, MD results have demonstrated
that the surface-driven stability of MoS2 structures can
be indicated by the desulfurization contents on one surface of MoS2 monolayer sheets, and the self-assembly of MoS2 monolayer sheets by desulfurization can emerge to adjust their surface-driven
stability. The study provides important atomic insights into tuning
the self-assembling structural morphologies of 2D materials through
defect engineering in the future science and engineering applications.