JCNS-1 and ICS-1, Forschungszentrum Jülich, Leo-Brandt-Straße, 52425 Jülich, Germany.
JCNS-SNS, Oak Ridge National Laboratory, Bethel Valley Road, Oak Ridge, Tennessee 37831, USA.
Phys Rev Lett. 2015 Sep 18;115(12):128302. doi: 10.1103/PhysRevLett.115.128302. Epub 2015 Sep 16.
We investigate the dynamics of kinetically frozen block copolymer micelles of different softness across a wide range of particle concentrations, from the fluid to the onset of glassy behavior, through a combination of rheology, dynamic light scattering, and pulsed field gradient NMR spectroscopy. We additionally perform Brownian dynamics simulations based on an ultrasoft coarse-grained potential, which are found to be in quantitative agreement with experiments, capturing even the very details of dynamic structure factors S(Q,t) on approaching the glass transition. We provide evidence that for these systems the Stokes-Einstein relation holds up to the glass transition; given that it is violated for dense suspensions of hard colloids, our findings suggest that its validity is an intriguing signature of ultrasoft interactions.
我们通过流变学、动态光散射和脉冲场梯度 NMR 光谱学的组合,研究了不同柔软度的动力学冻结嵌段共聚物胶束在广泛的粒子浓度范围内的动力学,从流体到玻璃行为的开始。我们还基于超软粗粒化势进行了布朗动力学模拟,发现这些模拟与实验结果非常吻合,甚至在接近玻璃转变时,对动态结构因子 S(Q,t)的细节也能进行很好的捕捉。我们提供的证据表明,对于这些体系,Stokes-Einstein 关系在玻璃转变之前是成立的;鉴于它在硬胶体的密集悬浮液中是被违反的,我们的发现表明,它的有效性是超软相互作用的一个有趣特征。