Abstract
Polymerization-induced self-assembly (PISA) has become widely recognized as a robust and efficient route to produce nanostructured systems toward functionally superior materials. Herein, by combining mesoscale simulations and micromechanical modeling, we report the structural control over the interfacial organization and the resulted micromechanical behaviors of novel nanocomposites designed based on the PISA of initiator-modified Janus nanoparticles in diblock copolymers. Our simulations demonstrate that the off-center distribution of these functionalized Janus nanoparticles with respect to phase interface can be precisely regulated by tuning the reaction kinetics and the concentration of monomers dispersed in polymer microdomains. Theoretical calculation reveals that such polymerization-induced interfacial self-assembly of Janus nanoparticles is fundamentally attributed to a unique entropy effect mediated by the reaction. The diffusion dynamics of monomers in the entanglement mesh of the diblock copolym...
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