Self-Assembly of Sequence-Defined Polymers Toward Materials Mimicking Living Systems – MimicLS

Creating synthetic polymer materials with the sophistication and complexity of living matter has been a long-term goal in materials science. In biological systems, self-assembly benefits from evolutionary optimization of molecular interactions that fine-tune the structure, morphology, and function of biomaterials. Nature uses the primary sequence of macromolecules (such as proteins) to direct folding into specific motifs, which then self-organize into complex, functional structures.

In contrast, synthetic polymers still lack the advanced hierarchical organization and functionalities seen in living systems. Therefore, from a materials innovation standpoint, it is essential to design well-defined interactions between building blocks that allow them to assemble into predetermined hierarchical architectures and exhibit diverse functionalities.

In recent years, peptide self-assembly has attracted significant attention. Although peptide-based materials with defined sequences have shown promise, their large-scale synthesis and rapid degradation remain major limitations. Sequence-defined abiotic polymers offer a solution to these challenges, adopting similar design strategies to peptides while providing greater stability and tunability. These polymers, defined by their precise primary structure, open new possibilities for next-generation synthetic materials that mimic biological organization. However, little is known about the single-chain folding of non-natural macromolecules or their self-assembly into complex supramolecular structures.

This collaborative project combines the expertise of two research teams:

• Functional Macromolecules Team, led by PhD Eng. Róża Szweda at Łukasiewicz – PORT, Poland, specializing in polymer science and self-assembly of sequence-defined polymer bioconjugates;

• Group of Prof. Takuji Adachi at the Faculty of Sciences, University of Geneva, Switzerland, specializing in optical spectroscopy and the development of in-situ spectroscopic tools to study self-assembly dynamics.

Together, the teams aim to investigate the fundamental self-assembly processes of abiotic, sequence-defined polymers. The goal is to gain a deeper understanding of sequence-regulated hierarchical polymer self-assembly, which is essential for designing synthetic materials with the structural sophistication and complexity of living systems.

The project encompasses three main research objectives:

1. Developing a synthesis method for high-molar-mass, sequence-defined polycarbamates using a mechanochemical approach.

2. Studying their self-assembly behavior in solution and solid states.

3. Characterizing the resulting material properties.

The research aims to determine how monomer sequence and stereochemistry influence aggregation into hierarchical structures, and how these structural differences affect rheological and thermal properties. Using in-situ microspectroscopy, the project will provide detailed insight into the mechanisms of polymer self-organization.

Understanding the relationship between molecular sequence and material properties will enable precise tuning of functionalities and serve as a powerful tool for the de novo design of functional, nature-inspired materials.