We apply a hybrid Molecular Dynamics and mesoscopic simulation technique to study the dynamics of two dimensional colloidal discs in confined geometries. We calculate the velocity autocorrelation functions, and observe the predicted $t^{-1}$ long time hydrodynamic tail that characterizes unconfined fluids, as well as more complex oscillating behavior and negative tails for strongly confined geometries. Because the $t^{-1}$ tail of the velocity autocorrelation function is cut off for longer times in finite systems, the related diffusion coefficient does not diverge, but instead depends logarithmically on the overall size of the system.
We investigate the tagged-particle motion in a strongly interacting quasi-confined liquid using periodic boundary conditions along the confining direction. Within a mode-coupling theory of the glass transition (MCT) we calculate the self-nonergodicity parameters and the self-intermediate scattering function and compare them with event-driven molecular dynamics simulations. We observe non-monotonic behavior for the in-plane mean-square displacement and further correlation functions which refer to higher mode indices encoding information about the perpendicular motion. The in-plane velocity-auto…
Bi-axial shear of confined colloidal suspensions: the structure and rheology of the vorticity-aligned string phase
利用一种新型的双轴共焦流变仪，我们研究了约束条件下剪切胶体悬浮液的结构和流变性。与以前的工作一致[X. Cheng \textit{et al., Proc. Natl. Acad. Sci. U. S. A.}，2011，109，63]，我们在单轴剪切下在中等浓度的胶体悬浮液中观察到涡旋对齐的弦相。使用双轴剪切协议，我们直接操纵的字符串结构的方向和形态。同时，我们使用双轴力测量装置测量了沿流动和涡度方向的悬浮液流变学。我们的研究结果表明，尽管高度各向异性的微观结构，悬浮液粘度保持各向同性和恒定的剪切速率探索。这些结果表明，流体动力学的贡献占主导地位的悬浮液响应。此外，他们强调双轴共焦流变仪的能力，阐明复杂流体的微观结构和流变学之间的关系。
The rotational Brownian motion of colloidal spheres in dense suspensions reflects local hydrodynamics and friction, both key to non-linear rheological phenomena such as shear-thickening and jamming, and transport in crowded environments, including intracellular migration and blood flow. To fully elucidate the role of rotational dynamics experimentally, it is crucial to measure the translational and rotational motion of all spheres simultaneously. Here, we develop compositionally uniform colloidal spheres with an off-centre, fully embedded core with a different fluorophore to the particle body,…
Dynamic heterogeneities and non-Gaussian behavior in two-dimensional randomly confined colloidal fluids
超顺磁性胶体颗粒的二元混合物被限制在玻璃板之间，使得大颗粒变得固定，并为仍然移动的小颗粒提供二维无序基质，其形成流体。通过改变流体和基质面积分数，并通过外部磁场调节超顺磁性颗粒之间的相互作用，探索了状态图的不同区域。移动粒子在小的基质面积分数下表现出离域动力学，在高的基质面积分数下表现出局域运动，并且局域化转变被软相互作用圆化[T. O. E. Skinner等人，Phys.Rev.Lett. { \bf 111}，128301（2013）]。扩展以前的工作，我们发现的动力学示踪剂是强烈的异质性，并表明，分子动力学模拟的理想气体局限在一个固定的矩阵表现出类似的行为。模拟显示了这些软相互作用如何使动力学比无序洛伦兹气体更不均匀，并导致强烈的非高斯波动。
We calculate the configurational entropy of colloidal particles in a confined geometry interacting as hard disks using Monte Carlo integration method. In particular, we consider systems with three kinds of boundary conditions: hard, periodic and spherical. For small to moderate packing fraction $ϕ$ values, we find the entropies per particle for systems with the periodic and spherical boundary conditions tend to reach a same value with the increase of the particle number $N$, while that for the system with the hard boundary conditions still has obvious differences compared to them within the st…
Based on Brownian dynamics simulations, we investigate the thermodynamic signatures of non-equilibrium steady states in a confined colloidal suspensions under shear flow. Specifically, we consider a thin film consisting of charged particles in narrow slit-pore confinement, forming two layers with quadratic in-plane structure in equilibrium. This many-body system displays three distinct steady states, characterized by unique dynamical and rheological response to the applied shear flow. Calculating the work and heat, we find that both quantities indicate the different states by their mean and by…
Drying dynamics of a charged colloidal dispersion in a confined drop
我们进行了彻底的调查，在一个封闭的几何形状的带电胶体分散液滴的干燥动力学。我们开发了一种基于拉曼显微光谱的原始方法来测量液滴干燥过程中的空间分辨胶体浓度分布。这些测量导致，第一次，估计的集体扩散系数的分散在很宽的范围内的浓度。集体扩散系数是一个数量级高于斯托克斯-爱因斯坦估计的浓度梯度的松弛的静电相互作用的重要性。与此同时，我们还进行了荧光成像的示踪剂嵌入分散液中的干燥过程中的下降，这揭示了两个不同的制度。在早期阶段，沿液滴的浓度梯度导致浮力诱导的流动。引人注目的是，这些流动并不影响产生它们的胶体浓度梯度，因为质量传递仍然由扩散主导。在较长的时间尺度上，示踪剂的轨迹揭示了准均匀干燥的凝胶的形成。对于这样的凝胶，我们表明使用线性孔隙弹性模型，干燥动力学仍然是由相同的传输方程描述的液体分散体。然而，集体扩散系数遵循修改的广义斯托克斯-爱因斯坦关系，如Style等人在单向固结的上下文中所证明的那样[Crust formation in drying colloidal suspension，Style等人，程序R. A 467，174（2011）]。
Active fluids comprise a variety of systems composed of elements immersed in a fluid environment which can convert some form of energy into directed motion; as such they are intrinsically out-of-equilibrium in the absence of any external forcing. A fundamental problem in the physics of active matter concerns the understanding of how the characteristics of the autonomous propulsion and agent-agent interactions determine the collective dynamics of the system. We study numerically suspensions of self-propelled diffusiophoretic colloids, in (quasi)-2d configurations, accounting for both dynamicall…
Strongly confined colloidal dispersions under shear can exhibit a variety of dynamical phenomena, including depinning transitions and complex structural changes. Here, we investigate the behaviour of such systems under pure oscillatory shearing with shear rate $\dotγ(t) = \dotγ_0 \cos(ωt)$, as it is a common scenario in rheological experiments. The colloids' depinning behaviour is assessed from a particle level based on trajectories, obtained from overdamped Brownian Dynamics simulations. The numerical approach is complemented by an analytic one based on an effective single-particle model in t…
Hydrodynamic interactions are important for diverse fluids especially those with low Reynold's number such as microbial and particle-laden suspensions, and proteins diffusing in membranes. Unfortunately, while far-field (asymptotic) hydrodynamic interactions are fully understood in two- and three-dimensions, near-field interactions are not, and thus our understanding of motions in dense fluid suspensions is still lacking. In this contribution, we experimentally explore the hydrodynamic correlations between particles in quasi-two-dimensional colloidal fluids in the near-field. Surprisingly, the…
Exploring the role of hydrodynamic interactions in spherically-confined drying colloidal suspensions
Auburn University（奥本大学）；Leibniz-Institut für Polymerforschung Dresden e.V.（德累斯顿莱布尼茨聚合物研究所）；Technische Universität Dresden（德累斯顿工业大学）；Johannes Gutenberg University Mainz（美因茨约翰内斯·古腾堡大学）
Effects of rigid or adaptive confinement on colloidal self-assembly. Fixed vs. fluctuating number of confined particles
在[J. Pakkalski et al. J. Chem. Phys. 142，014903（2015）]中的大正则方程组（GCE）中精确求解的一维晶格模型中，研究了在固定数量的受限粒子的情况下，受限对胶体自组装的影响。该模型考虑了由短程吸引加上长程排斥定义的对相互作用。我们考虑与自组装成团簇相对应的热力学状态。固定和自适应边界进行了研究。对于固定的边界，有一些特殊的状态，在这些状态中，对于相等的平均密度，GCE中的团簇数量大于正则包围圈中的团簇数量。当系统尺寸随颗粒数的变化而变化时，压力对密度的依赖关系与当颗粒数随系统尺寸的变化而变化时有不同的形式。在前一种情况下，压力对系统尺寸有非单调的依赖关系。膨胀系统压力的异常增加伴随着大量小团簇的形成。在弹性约束面的情况下，我们观察到一个双稳态，即两个显着不同的系统大小发生几乎相同的概率。在封闭系统中的双稳态的机制是不同的情况下的渗透壁，其中两个平衡系统的大小对应于不同数量的颗粒。
We study self-diffusion and sedimentation in colloidal suspensions of nearly-hard spheres using the multiparticle collision dynamics simulation method for the solvent with a discrete mesh model for the colloidal particles (MD+MPCD). We cover colloid volume fractions from 0.01 to 0.40 and compare the MD+MPCD simulations to Brownian dynamics simulations with free-draining hydrodynamics (BD) as well as pairwise far-field hydrodynamics described using the Rotne--Prager--Yamakawa mobility tensor (BD+RPY). The dynamics in MD+MPCD suggest that the colloidal particles are only partially coupled to the…
The complex behavior of confined fluids arising due to a competition between layering and local packing can be disentangled by considering quasi-confined liquids, where periodic boundary conditions along the confining direction restore translational invariance. This system provides a means to investigate the interplay of the relevant length scales of the confinement and the local order. We provide a mode-coupling theory of the glass transition (MCT) for quasi-confined liquids and elaborate an efficient method for the numerical implementation. The nonergodicity parameters in MCT are compared to…
The hydrodynamic resistance matrix is an important quantity for describing the dynamics of colloidal particles. This matrix encodes the shape- and size-dependent hydrodynamic properties of a particle suspended in a simple liquid at low Reynolds number and determines the particle's diffusion tensor. For this reason, the hydrodynamic resistance matrix is typically needed when modeling the motion of free purely Brownian, externally driven, or self-propelled colloidal particles or the behavior of dilute suspensions of such particles on the basis of Langevin equations, Smoluchowski equations, class…
We present numerical results for the tagged-particle dynamics by solving the mode-coupling theory in confined geometry for colloidal liquids (cMCT). We show that neither the microscopic dynamics nor the type of intermediate scattering function qualitatively changes the asymptotic dynamics in vicinity of the glass transition. In particular, we find similar characteristics of confinement in the low-frequency susceptibility spectrum which we interpret as footprints of parallel relaxation. We derive predictions for the localization length and the scaling of the diffusion coefficient in the superco…
