The effect of electrostatic interactions on the critical percolation concentration (c(p)) of fibrillar beta-lactoglobulin gels at pH 2 was investigated using rheological measurements, transmission electron microscopy (TEM), and performing conversion experiments. A decreasing c(p) with increasing ionic strength was found. The fraction of nonaggregated beta-lactoglobulin was independent of ionic strength in the regime of 0.01-0.08 M. TEM experiments showed long fibrils (2-7 microm) for ionic strengths between 0.01 and 0.08 M. Since both the conversion of monomers and the contour length of the fibrils were independent of ionic strength (0.01-0.08M), the linear increase of c(p) with the Debye length can be attributed purely to an increase of electrostatic repulsion between the fibrils. This increase is explained in terms of an adjusted random contact model which takes into account the charge and semiflexibility of the fibrils.
Relaxation of flow birefringence can give a direct measure of the rotational diffusion of rodlike objects in solution. With a suitable model of the rotational diffusivity, a length distribution can be sought by fitting the decay curve. We have measured the flow birefringence decay from solutions of amyloid fibrils composed of β-lactoglobulin and extracted a length distribution using the Doi-Edwards-Marrucci-Grizzuti theory of semidilute rotational diffusion. The concentration scaling of the results shows that the fibrils diffuse as free rods: they cannot be significantly branched, sticky, or break up under dilution. The length distribution obtained shows a single broad peak, consistent with measurements of the fibrils by electron microscopy. This comparison, and combination of the experiment with an assay to find the total concentration of fibrils, allows calibration of the length scale and concentration scale of the length distribution. It is our hope that this method can be used for following the growth kinetics of amyloid fibrils in vitro and for studying the length distribution of rodlike systems in general.
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