Fortini Andrea, Sanz Eduardo, Dijkstra Marjolein
Debye Institute for NanoMaterials Science, Utrecht University, Princetonplein 5, 3584 CC Utrecht, The Netherlands.
Phys Rev E Stat Nonlin Soft Matter Phys. 2008 Oct;78(4 Pt 1):041402. doi: 10.1103/PhysRevE.78.041402. Epub 2008 Oct 3.
We systematically study the relationship between equilibrium and nonequilibrium phase diagrams of a system of short-ranged attractive colloids. Using Monte Carlo and Brownian dynamics simulations we find a window of enhanced crystallization that is limited at high interaction strength by a slowing down of the dynamics and at low interaction strength by the high nucleation barrier. We find that the crystallization is enhanced by the metastable gas-liquid binodal by means of a two-stage crystallization process. First, the formation of a dense liquid is observed and second the crystal nucleates within the dense fluid. In addition, we find at low colloid packing fractions a fluid of clusters, and at higher colloid packing fractions a percolating network due to an arrested gas-liquid phase separation that we identify with gelation. We find that this arrest is due to crystallization at low interaction energy and it is caused by a slowing down of the dynamics at high interaction strength. Likewise, we observe that the clusters which are formed at low colloid packing fractions are crystalline at low interaction energy, but glassy at high interaction energy. The clusters coalesce upon encounter.
我们系统地研究了短程吸引胶体系统的平衡相图和非平衡相图之间的关系。通过蒙特卡罗模拟和布朗动力学模拟,我们发现了一个增强结晶的窗口,在高相互作用强度下,该窗口受到动力学减慢的限制,而在低相互作用强度下,则受到高成核势垒的限制。我们发现,亚稳气液双节线通过两阶段结晶过程增强了结晶。首先,观察到形成了致密液体,其次,晶体在致密流体中形核。此外,我们发现在低胶体填充分数下是团簇流体,而在较高胶体填充分数下,由于我们确定为凝胶化的气液相分离受阻而形成渗流网络。我们发现这种受阻在低相互作用能下是由于结晶,而在高相互作用强度下是由动力学减慢引起的。同样,我们观察到在低胶体填充分数下形成的团簇在低相互作用能下是晶体,但在高相互作用能下是玻璃态。团簇相遇时会合并。