The control of the self-assembly of the nanocrystals into ordered
structures has been extensively investigated, but fewer efforts have
been devoted to studying one-component polymer-grafted nanoparticles
(OPNPs). Herein, through coarse-grained molecular dynamics simulation,
we design a novel nanoparticle (NP) grafted with polymer chains, focusing
on its self-assembled structures. First, we examine the effects of
length and density of grafted polymer chains by calculating the radial
distribution function between NPs, as well as through direct visualization.
We observe a monotonic change of the arranged morphology of grafted-NPs
as a function of the density of grafted polymer chains, which indicates
that the increase of the grafting density contributes to the order
of the morphology. Meanwhile, we find that much longer grafted polymer
chains worsen the regularity of the morphology. Then, we probe the
influence of the stiffness of grafted polymer chains (denoted by K ranging from 0 to 500) on the order of grafted-NPs, finding
that the order of the structure exhibits a nonmonotonic behavior as
a function of K at moderate grafting density. For
high grafting density, the order of the morphology is initially enhanced
and becomes saturated as a function of K. For the
effect of K on the stress–strain behavior,
the system with the lowest order demonstrates the most remarkable
reinforced mechanical behavior for both low and high grafting density.
Last, we establish the phase diagram by varying the stiffness and
density of the grafted polymer chains, which contains the amorphous,
ordered, and superlattice structures, respectively. In general, our
simulated results provide guidelines to tailor the self-assembly of
the OPNPs by taking advantage of the length, density, and stiffness
of grafted polymer chains.