Gelation dynamics upon pressure-induced liquid-liquid phase separation in a water-lysozyme solution

Abstract

Employing X-ray photon correlation spectroscopy we measure the kinetics and dynamics of a pressure-induced liquid-liquid phase separation (LLPS) in a water-lysozyme solution. Scattering invariants and kinetic information provide evidence that the system reaches the phase boundary upon pressure-induced LLPS with no sign of arrest. The coarsening slows down with increasing quench depths. The $g_2$-functions display a two-step decay with a gradually increasing non-ergodicity parameter typical for gelation. We observe fast superdiffusive (${\hat{I}}^3\ge 3/2$) and slow subdiffusive (${\hat{I}}^3<0.6$) motion associated with fast viscoelastic fluctuations of the network and a slow viscous coarsening process, respectively. The dynamics age linear with time $\ddot{I}„\propto t_{\mathrm{w}}$ and we observe the onset of viscoelastic relaxation for deeper quenches. Our results suggest that the protein solution gels upon reaching the phase boundary.