Van der Waals-Zeeman Institute, Institute of Physics, Science Park 904, 1098 XH Amsterdam, The Netherlands.
School of Mathematics, University of Bristol, Bristol BS8 1TW, United Kingdom.
J Chem Phys. 2018 Feb 14;148(6):064901. doi: 10.1063/1.4990101.
Homogeneous crystal nucleation from a metastable hard-sphere colloidal liquid has been extensively studied in simulations and experiments. A 12 order of magnitude difference between simulated and experimental nucleation rates is observed, the origin of which remains a puzzle. Here, we experimentally study crystal nucleation at the single particle level in suspensions of hard-sphere-like colloids under the influence of sedimentation. We find that sedimentation significantly enhances the nucleation rate, but contrary to what was previously thought, this is not due to simple density fluctuations, as the nucleation barriers become independent of the local density in a sedimentating fluid. Instead, we find an enhancement of the local dynamics, which suggests that local convective cells are responsible for shear-enhanced crystallization at low volume fractions.
从亚稳硬球胶体液体中进行均相成核已在模拟和实验中得到广泛研究。在模拟和实验成核率之间观察到 12 个数量级的差异,其起源仍然是一个谜。在这里,我们在硬球胶体悬浮液中单颗粒水平下研究了沉降作用下的晶体成核。我们发现,沉降显著提高了成核速率,但与之前的想法相反,这并不是由于简单的密度涨落,因为成核势垒与沉降流体中的局部密度无关。相反,我们发现局部动力学增强,这表明在低体积分数下局部对流单元负责剪切增强结晶。