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Time‐Resolved study of network self‐organization from a biopolymeric solution

Time‐resolved studies of network self‐organization from homogeneous solutions of the representative biostructural polymer agarose are presented. Solutions are temperature quenched and observed by several techniques. Consistent with previous suggestions by the authors, experiments at concentrations up to about 1.75% w/v provide direct kinetic evidence for the occurrence of at least two distinct processes, leading, in sequence, to self‐assembly. These are as follows: (a) a liquid–liquid phase separation of the solution occurring via spinodal demixing and resulting in two sets of regions that have, respectively, higher and lower than average concentrations of random‐coiled polymers; and (b) the subsequent 2 coils → double helix transition and accompanying cross‐linking and gelation (due to branching of double helices), occurring in the high‐concentration regions. The size of the high‐concentration regions depends upon agarose concentration and quenching temperature, and is in the range from a fraction of micrometers to a few micrometers, in agreement with earlier experiments. Bundling of the double‐helical segments is known to follow self‐assembly and can be considered as a third step (gel curing). This follows from the thermo‐dynamic instability of the helical segments in the solvent, behaving as a system of rod‐like particles connected by more or less flexible joints.