论文标题
订购与剪切稀疏之间的相关性
Correlation between ordering and shear thinning in confined liquids
论文作者
论文摘要
尽管数十年来一直在对限制液体的行为进行了广泛的研究,但对这种现象的详细知识,尤其是在混合/边界润滑方案中,仍然有限。这可以归因于几个因素,包括在非平衡条件下直接观察润滑剂分子行为的难度,分子模拟的高计算成本达到稳态,以及在与实际操作条件相对应的极低剪切速率下的信噪比低。为此,我们研究了在混合/边界润滑状态下两个云母表面之间的八甲基环甲氧烷的结构形成与剪切粘度之间的相关性。考虑到对应于两层,三层和五层结构的三个不同的表面分离来分析限制的影响。在休息时观察到具有$ n = 2 $的一个特定峰的定向分布,包括与$ n> 2 $的平行定向。限制的液体表现出独特的剪切行为,独立于表面分离,对于相对较低的滑动速度,$ v _ {\ rm x} \ Lessim 10^{ - 1} \,{\ rm m/s} $。但是,$ v _ {\ rm x} \ sillsim 10^{ - 1} \,{\ rm m/s} $的剪切粘度取决于分层结构的数量。观察到牛顿行为,滑动速度进一步增加。此外,我们发现分子取向程度与受限液体的剪切粘度之间存在很强的相关性。受限液体的剪切粘度的大小可以主要取决于分子取向的程度,而剪切薄的含量源自特定定向分布的消失,而滑动速度的增加。
Despite the extensive research that has been conducted for decades on the behavior of confined liquids, detailed knowledge of this phenomenon, particularly in the mixed/boundary lubrication regime, remains limited. This can be attributed to several factors including the difficulty of direct experimental observations of the behavior of lubricant molecules under non-equilibrium conditions, the high computational cost of molecular simulations to reach steady state, and the low signal-to-noise ratio at extremely low shear rates corresponding to actual operating conditions. To this end, we studied the correlation between the structure formation and shear viscosity of octamethylcyclotetrasiloxane confined between two mica surfaces in a mixed/boundary lubrication regime. Three different surface separations corresponding to two-, three-, and five-layered structures were considered to analyze the effect of confinement. The orientational distributions with one specific peak for $n=2$ and two distributions, including a parallel orientation with the surface normal for $n>2$, were observed at rest. The confined liquids exhibited a distinct shear-thinning behavior independent of surface separations for a relatively low sliding velocity, $V_{\rm x}\lesssim 10^{-1}\,{\rm m/s}$. However, the shear viscosities at $V_{\rm x}\lesssim 10^{-1}\,{\rm m/s}$ depended on the number of layered structures. Newtonian behavior was observed with a further increase in the sliding velocity. Furthermore, we found a strong correlation between the degree of molecular orientation and the shear viscosity of the confined liquids. The magnitude of the shear viscosity of the confined liquids can primarily be determined by the degree of molecular orientation, and shear-thinning originates from the vanishing of specific orientational distributions with increasing sliding velocity.