Dissipative structures in proteoglycan solutions.

Diffusion in multicomponent solutions containing proteoglycan is shown to result in the formation of coherent, fluid structures (known as dissipative structures) and induction of rapid polymer transport. These phenomena occur over a wide range of conditions (i.e. varying solute distribution, concentration, size, and chemical composition) which are envisaged to occur in the extracellular matrix of connective tissues. A concentration gradient of chondroitin sulfate in a proteoglycan matrix of uniform concentration yields dissipative structures which transport the proteoglycan up to 300-fold faster than its transport in the absence of the gradient component. Similar behavior was observed with other polysaccharide and monosaccharide concentration gradient components. Amplification of structure formation and rapid transport was achieved by 1) increasing the concentration of proteoglycan matrix, 2) increasing the magnitude of the concentration gradient, 3) decreasing the molecular weight of the gradient-forming component, and 4) decreasing the concentration gradient of proteoglycan in the matrix. Dissipative structure morphology exhibits a marked dependence on the initial component distribution. Non-specific, excluded volume interactions between the proteoglycan and the gradient component are believed to induce coupled diffusive transport of the proteoglycan. This leads to microscopic density inversions which nucleate and develop into macroscopic convective flows. These results are similar to those previously observed in ternary solutions of uncharged polymers (i.e. dextran/polyvinylpyrrolidone). We have demonstrated that dissipative structures may transport Micrococcus luteus cells as well as various solutes. Flows were also observed in proteoglycan solutions after localized addition of small amounts of either a proteolytic enzyme or hyaluronic acid. It is likely that the prerequisites for this spontaneous macroscopic self-organization, as manifested by the flow phenomenon, are present in the extracellular matrix of connective tissues.