Crystal-Arrested Phase Separation

We have studied the interplay between phase separation and crystallization in a colloid-polymer mixture along one kinetic pathway in samples which exhibit three-phase equilibrium coexistence. In analogy with atomic systems, the range of the effective attractive interaction between colloids is sufficiently long to allow for a stable liquid phase. By direct imaging in microgravity on the International Space Station, we observe a unique structure, a "crystal gel," that occurs when gas-liquid phase separation arrests due to crystallites within the liquid domain spanning the cell. From the initial onset of spinodal decomposition until arrest caused by this structure, the kinetics of phase separation remain largely unaffected by the formation of the third phase. This dynamic arrest appears to result from the stiffness of the crystalline strands exceeding the liquid-gas interfacial tension.