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The phase behavior of polydisperse ABA triblock copolymers is studied usingdissipative particle dynamics simulations, focusing on the emergence andproperty of bicontinuous structures. Bicontinuous structures are characterizedby two separate, intermeshed nanoscopic domains extending throughout thematerial. The connectivity of polymeric bicontinuous structures makes themhighly desirable for many applications. For conventional monodisperse diblockand triblock copolymers, regular bicontinuous structures (i.e., gyroid andFddd) can be formed over a narrow composition window of ~3%. We demonstratethat the composition window for the formation of bicontinuous structures can beregulated by designed polydispersity distributions of ABA triblock copolymers.In particular, introducing polydispersity in both A and B blocks can lead to asignificant enhancement of the composition window of bicontinuous structureswith both continuous A and B domains. The mechanism of the bicontinuousstructure enhancement is elucidated from the distribution of the long and shortblocks. Furthermore, it is shown that the polymeric bicontinuous structuresfrom polydisperse ABA triblock copolymers possess good continuity throughoutthe sample, making them ideal candidates for advanced applications.

Enhancing Composition Window of Bicontinuous Structures by Designed Polydispersity Distribution of ABA Triblock Copolymers