Re-entrant isotropic-nematic phase behavior in polymer-depleted amyloid fibrils

Amyloid fibrils dispersed in water exhibit both isotropic (I) and nematic (N) phases, depending on concentration, but their coexistence, expected from the first order nature of the I − N thermodynamic transition is seldom observed. By adding a non-absorbing polymer to an amyloid fibrils suspension, we report, for the first time, an unusual closed-loop phase behavior. The phase diagrams reveal that the I + N coexistence does emerge, but only when the depleting polymer is present at intermediate concentrations. We combine depletion potentials in the dilute and semi-dilute polymer regime with the DLVO theory and the principle of equivalent law of corresponding states to calculate variations of the second virial coefficient with increasing polymer concentrations. We conclude that the decrease of the depletion potential range in the semi-dilute regime plays a pivotal role in the observed re-stabilization, leading to a closure of the I + N coexistence region.