Abstract
Correlating the structures and properties of a polymer to its monomer sequence is key to understanding how its higher hierarchy structures are formed and how its macroscopic material properties emerge. Carbohydrate polymers, such as cellulose and chitin, are the most abundant materials found in nature whose structures and properties have been characterized only at the submicrometer level. Here, by imaging single-cellulose chains at the nanoscale, we determine the structure and local flexibility of cellulose as a function of its sequence (primary structure) and conformation (secondary structure). Changing the primary structure by chemical substitutions and geometrical variations in the secondary structure allow the chain flexibility to be engineered at the single-linkage level. Tuning local flexibility opens opportunities for the bottom-up design of carbohydrate materials.
Highlights
Correlating the structures and properties of a polymer to its monomer sequence is key to understanding how its higher hierarchy structures are formed and how its macroscopic material properties emerge
By examining the local freedom of the chain as a function of its primary and secondary structures, we address how low-hierarchy structural motifs affect local oligosaccharide flexibility—an insight critical to the bottom-up design of carbohydrate materials [30]
Modified analogs prepared by Automated Glycan Assembly (AGA) [11, 12] were designed to manipulate particular intramolecular interactions responsible for cellulose flexibility
Summary
Correlating the structures and properties of a polymer to its monomer sequence is key to understanding how its higher hierarchy structures are formed and how its macroscopic material properties emerge. We use this technique to correlate the local flexibility of an oligosaccharide chain to its sequence and conformation, the lowest two structural hierarchies. We establish the structure–property relationship for a polysaccharide at the atomic level by determining molecular flexibility of carbohydrate chains with defined sequences. The chain flexibility can be engineered one linkage at a time by chemical substitution and conformation change, highlighting how the primary and secondary structures of a carbohydrate dictate its flexibility—a critical observable in the de novo design of carbohydrate materials.
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