Das Sayan, Jalilvand Zohreh, Popescu Mihail N, Uspal William E, Dietrich Siegfried, Kretzschmar Ilona
Max-Planck-Institut für Intelligente Systeme, Heisenbergstr. 3, D-70569 Stuttgart, Germany.
Department of Chemical Engineering, City College of the City University of New York (CUNY), 140th Street and Convent Avenue, New York, New York 10031, United States.
Langmuir. 2020 Jun 30;36(25):7133-7147. doi: 10.1021/acs.langmuir.9b03696. Epub 2020 Feb 10.
Chemically active particles achieve motility without external forces and torques ("self-propulsion") due to catalytic chemical reactions at their surfaces, which change the chemical composition of the surrounding solution (called "chemical field") and induce hydrodynamic flow of the solution. By coupling the distortions of these fields back to its motion, a chemically active particle experiences an effective interaction with confining surfaces. This coupling can lead to a rich behavior, such as the occurrence of wall-bound steady states of "sliding". Most active particles are density mismatched with the solution and, thus, tend to sediment. Moreover, the often employed Janus spheres, which consist of an inert core material decorated with a cap-like, thin layer of a catalyst, are gyrotactic (i.e., "bottom-heavy"). Whether or not they may exhibit sliding states at horizontal walls depends on the interplay between the active motion and the gravity-driven sedimentation and alignment, such as the gyrotactic tendency to align the axis along the gravity direction being overcome by a competing, activity-driven alignment with a different orientation. It is therefore important to understand and quantify the influence of these gravity-induced effects on the behavior of model chemically active particles moving in the vicinity of walls. For model gyrotactic, self-phoretic Janus particles, here we study theoretically the occurrence of sliding states at horizontal planar walls that are either below ("floor") or above ("ceiling") the particle. We construct "state diagrams" characterizing the occurrence of such states as a function of the sedimentation velocity and of the gyrotactic response of the particle, as well as of the phoretic mobility of the particle. We show that in certain cases sliding states may emerge at both the ceiling and the floor, while the larger part of the experimentally relevant parameter space corresponds to particles that would exhibit sliding states only either at the floor or at the ceiling-or there are no sliding states at all. These predictions are critically compared with the results of previous experimental studies, as well as with our dedicated experiments carried out with Pt-coated, polystyrene-core, or silica-core Janus spheres immersed in aqueous hydrogen peroxide solutions.
由于其表面的催化化学反应,化学活性粒子在没有外力和扭矩的情况下实现运动(“自推进”),这种反应会改变周围溶液的化学成分(称为“化学场”)并引发溶液的流体动力流动。通过将这些场的畸变反馈到其运动中,化学活性粒子会与限制表面产生有效相互作用。这种耦合会导致丰富的行为,例如出现“滑动”的壁面束缚稳态。大多数活性粒子与溶液的密度不匹配,因此容易沉降。此外,常用的 Janus 球由惰性核心材料和帽状的薄催化剂层组成,具有趋旋光性(即“头重脚轻”)。它们在水平壁上是否会呈现滑动状态取决于主动运动与重力驱动的沉降和排列之间的相互作用,例如沿重力方向排列轴的趋旋光倾向是否会被另一种不同方向的、由活性驱动的排列所克服。因此,了解和量化这些重力诱导效应对在壁附近运动的模型化学活性粒子行为的影响非常重要。对于模型趋旋光、自泳 Janus 粒子,我们在此从理论上研究了在粒子下方(“地板”)或上方(“天花板”)的水平平面壁上滑动状态的出现情况。我们构建了“状态图”,将此类状态的出现情况表征为沉降速度、粒子的趋旋光响应以及粒子的自泳迁移率的函数。我们表明,在某些情况下,天花板和地板处都可能出现滑动状态,而实验相关参数空间的大部分对应于仅在地板或天花板处呈现滑动状态的粒子——或者根本不存在滑动状态。这些预测与先前实验研究的结果以及我们用浸入过氧化氢水溶液中的铂涂层、聚苯乙烯核心或二氧化硅核心的 Janus 球进行的专门实验结果进行了严格比较。