Scientists have developed photoresponsive supramolecular polymers that can undergo both intrachain folding and interchain aggregation.
The material properties of polymers are determined by the competition between polymer chain folding and aggregation. For the first time, researchers from Japan developed folded supramolecular polymers that can spontaneously undergo interchain aggregation. Using atomic force microscopy, they revealed that this interchain aggregation proceeded through the unfolding of the main chains.
"Originally, we found a monomer structure that polymerized in a spiral shape. This time, we partially changed the structure of the unit that drives the polymerization of the monomer to investigate the monomer-polymer relationship. To our surprise, we observed a phenomenon where the spiral spontaneously unfolds, and the different chains bundle together.
Furthermore, the team revealed the reason behind this structural transformation. This included intrachain molecular ordering due to conformational changes in the biphenyl unit and interchain ordering from the alignment of the aliphatic tails covering the exterior of the main chains. This mechanism is similar to the crystallization of conventional covalent polymers. The team corroborated this mechanism using the photoisomerization of the azobenzene unit.
"These phenomena have traditionally been investigated using spectroscopic or macroscopic observations, reflecting the averaged behavior of the whole system. Therefore, the construction of more observable mesoscale models is expected to contribute significantly to the advancement of materials science. We are hopeful that these insights can encourage the development of meso-scale molecular assemblies with meaningful higher-order structures," concluded Prof. Yagai.
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