Labalette Vincent, Praga Alexis, Girard Florent, Meireles Martine, Hallez Yannick, Morris Jeffrey F
Laboratoire de Génie Chimique, Université de Toulouse, CNRS, INPT, UPS, Toulouse, France.
Soft Matter. 2021 Mar 21;17(11):3174-3190. doi: 10.1039/d0sm02081h. Epub 2021 Feb 23.
A new numerical framework based on Stokesian dynamics is used to study a shear-induced glass-to-crystal transition in suspensions of clay-like anisotropically charged platelets. The structures obtained in quiescent conditions are in agreement with previous Monte Carlo results: a liquid phase at very short interaction range (high salt concentration), phase separation and a gel without large scale density fluctuations at intermediate interaction ranges, and glassy states at very large interaction ranges. When initially glassy suspensions are sheared, hydrodynamic torques first rotate platelets so they can reach a transient quasi-nematic disordered state. These orientational correlations permit to unlock translational degrees of freedom and the platelets then form strings aligned with the velocity direction and hexagonally packed in the gradient-vorticity plane. Under steady shear, platelet orientations are correlated but the system is not nematic. After flow cessation and relaxation in quiescent conditions, positional and orientational order are further improved as the platelet suspension experiences a transition to a nematic hexagonal crystal. Energy calculations and the existence of residual stress anisotropy after relaxation show that this final structure is not an equilibrium state but rather a new ordered, arrested state. The transient, nematic, disordered state induced by shear immediately after startup and unlocking translational degrees of freedom is thought to be an initial step that may be generic for other suspensions of strongly anisotropic colloids with important translation-orientation coupling induced by long-range interactions.
一种基于斯托克斯动力学的新数值框架被用于研究黏土状各向异性带电薄片悬浮液中剪切诱导的玻璃态到晶态的转变。在静态条件下获得的结构与先前的蒙特卡罗结果一致:在非常短的相互作用范围(高盐浓度)下为液相,在中间相互作用范围内发生相分离且形成无大规模密度涨落的凝胶,在非常大的相互作用范围内为玻璃态。当初始处于玻璃态的悬浮液受到剪切时,流体动力扭矩首先使薄片旋转,使其能够达到瞬态准向列无序状态。这些取向相关性允许释放平动自由度,然后薄片形成与速度方向对齐并在梯度 - 涡度平面中呈六边形堆积的链。在稳定剪切下,薄片取向相关,但系统并非向列相。在停止流动并在静态条件下弛豫后,随着薄片悬浮液经历向列六边形晶体的转变,位置和取向有序性进一步提高。能量计算以及弛豫后残余应力各向异性的存在表明,这种最终结构不是平衡态,而是一种新的有序的、停滞态。启动后剪切立即诱导的瞬态、向列、无序状态以及释放平动自由度被认为是一个初始步骤,对于其他具有由长程相互作用引起的重要平动 - 取向耦合的强各向异性胶体悬浮液可能是通用的。