A new mesophase in binary blends
of A–b–(BA′)3 miktoarm star block
copolymers and A homopolymers has recently
been discovered experimentally and explored with field-theoretic simulations.
This mesophase has been reported to consist of aperiodic discrete
domains of A embedded in a continuous matrix of B up to very high
concentrations of A. Because of the material’s potential as
a thermoplastic elastomer, a deeper understanding of its structural
and dynamic-mechanical properties, including its domain connectivity,
linear rheological behavior, response to shear, and response to uniaxial
tension, is warranted. These properties are explored here using dissipative
particle dynamics in three dimensions, for the first time. These simulations
establish that the so-called “bricks-and-mortar” phase,
while appearing discrete in two dimensions, is bicontinuous. The simulations
focusing on dynamics establish that the role of molecular bridging
dominates the mechanical behavior and outweighs the influence of microphase
segregation (contributions from the interfacial tension alone) even
at the highest homopolymer concentrations we study. Additionally,
it appears that the bricks-and-mortar phase is sensitive to the application
of sufficiently high shear, leading to nonisotropic mechanical responses,
which has ramifications for the processability of such materials.
We find that upon application of shear the phase becomes closer in
structure to its speculated discrete nature. Molecular simulations
on our longest accessible timescales show that the material is unable
to relax back to its original structure, suggesting that the morphology
observed depends heavily on the material process pathway.