Correlation of Structure and Dynamics Behavior in Polyzwitterions: From Concentrated Solution to Gel-Like State

The dynamic behaviors of polyzwitterions, poly(4-((3-methacrylamidopropyl) dimethylammonio) butane-1-sulfonate) (PSBP), are investigated using dynamic light scattering, small angle X-ray scattering, and rheology.  The findings reveal two relaxation modes, including a fast and a slow mode, which  are observed in both solution state and gel-like state, with varying polyzwitterion concentration (C_P ) and NaCl concentration (C_NaCl ). As C_P and C_NaCl increasing, a slower slow mode and a faster fast mode are observed. The fast mode corresponds to the diffusion of chains, while the slow mode arises from chain aggregations. In solutions, the slow mode is dominated by the diffusion of chain aggregations. However, in the gel-like state, the "cage network" traps aggregations more densely, leading to their dynamic behavior being dominated by enhanced topological entanglements and ionic interactions. This difference highlights the unique nature of the slow relaxation mode between concentrated solution and gel-like state, arising from changes in the average distance between chain aggregations resulting from increased C_P and C_NaCl concentrations.