Spontaneous long-range structural ordering of polymers can lead to improvements in their physical properties and the emergence of functions that cannot be expected in their amorphous states. We have demonstrated a design strategy to achieve structuring of various polymers using a particular type of triptycene, capable of forming a two-dimensional assembly. In this study, we investigated what designs are effective for achieving long-range polymer ordering by incorporating this triptycene motif into the side chains of polymers. Using poly(n-butyl acrylate) as a fundamental polymer, we synthesized three types of copolymers, i.e., random, diblock, and ABA-type triblock copolymers, through RAFT polymerization protocols and found that the presence of block segments is essential to achieve polymer ordering, which in turn results in dramatically improved mechanical properties. Here, we also show that poly(N-isopropylacrylamide)-based copolymers with triptycene-containing side chains undergo an interesting anisotropic expansion and contraction microscopically in response to temperature.
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