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Short- and long-time diffusion, and dynamic scaling in suspensions of charged colloidal particles

机译:短时和长时扩散,以及悬浮液中的动态缩放   带电的胶体颗粒

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摘要

We report on a comprehensive theory-simulation-experimental study ofcollective and self-diffusion in suspensions of charge-stabilized colloidalspheres. In simulation and theory, the spheres interact by a hard-core plusscreened Coulomb pair potential. Intermediate and self-intermediate scatteringfunctions are calculated by accelerated Stokesian Dynamics simulations wherehydrodynamic interactions (HIs) are fully accounted for. The study spans therange from the short-time to the colloidal long-time regime. Additionally,Brownian Dynamics simulation and mode-coupling theory (MCT) results aregenerated where HIs are neglected. It is shown that HIs enhance collective andself-diffusion at intermediate and long times, whereas at short timesself-diffusion, and for certain wavenumbers also collective diffusion, areslowed down. MCT significantly overestimate the slowing influence of dynamicparticle caging. The simulated scattering functions are in decent agreementwith our dynamic light scattering (DLS) results for suspensions of chargedsilica spheres. Simulation and theoretical results are indicative of along-time exponential decay of the intermediate scattering function. Theapproximate validity of a far-reaching time-wavenumber factorization of thescattering function is shown to be a consequence of HIs. Our study ofcollective diffusion is amended by simulation and theoretical results for theself-intermediate scattering function and the particle mean squareddisplacement (MSD). Since self-diffusion is not assessed in DLS measurements, amethod to deduce the MSD approximately in DLS is theoretically validated.
机译:我们报告了电荷稳定的胶体球悬浮液中的集体和自我扩散的综合理论模拟实验研究。在模拟和理论上,球体通过加硬核加库仑对势相互作用。中间和自中间散射函数是通过加速的斯托克斯动力学模拟计算出来的,其中充分考虑了流体动力相互作用(HIs)。研究范围从短时到胶体长时。此外,在忽略HI的情况下,会生成布朗动力学仿真和模式耦合理论(MCT)结果。结果表明,HIs在中长期内增强了集体和自我扩散,而在短时间内,自我扩散以及某些波数的集体扩散也减慢了。 MCT大大高估了动态粒子笼罩的影响。模拟的散射函数与带电二氧化硅球的悬浮液的动态光散射(DLS)结果非常吻合。仿真和理论结果表明中间散射函数随时间呈指数衰减。散射函数的远期波数分解的近似有效性被证明是HI的结果。通过对自中间散射函数和粒子均方位移(MSD)的仿真和理论结果对我们对集体扩散的研究进行了修正。由于在DLS测量中未评估自扩散,因此在理论上验证了在DLS中近似推论MSD的方法。

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