Interfacial Layer Breaker: A Violation of Stokes' Law in High-Speed Atomic Force Microscope Flows.
Interfacial Layer Breaker: A Violation of Stokes' Law in High-Speed Atomic Force Microscope Flows.
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DOI：
10.1021/acs.langmuir.2c02418
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发表时间：
2023-01-10
期刊：
影响因子：
3.9
通讯作者：
Karabasov, Sergey
中科院分区：
文献类型：
--
作者：
Li, Fan;Smoukov, Stoyan K.;Korotkin, Ivan;Taiji, Makoto;Karabasov, Sergey
表面附近的结构水在细胞膜的非经典结晶、生物矿化和重组中非常重要。除了原子力显微镜研究的平衡结构外，高速原子力显微镜(H-S原子力显微镜)现在可以在微秒内探测皮牛力。随着速度的增加和尖端直径的减小，存在着连续体水模型不适用的危险，需要分子动力学(MD)模拟来进行准确的预测。然而，由于内存和计算效率/速度的限制，MD模拟只能在几十纳秒内进化，因此需要新的方法来弥合这一差距。在这里，我们报告了一种混合的多尺度模拟方法，它可以弥合现有实验在大小和时间尺度上的差距。研究了移动的二氧化硅原子力显微镜胶体尖端和解理的云母表面之间的结构水。计算领域包括1,472,766个原子。当原子力显微镜针尖以5×10-7到30m/S的速度移动时，为了模拟水中发生的远程水动力的影响，采用了一种具有局部原子分辨率的混合多尺度方法作为有效的开域边界条件。因此，多尺度模拟相当于使用具有平衡边界条件的宏观大计算区域。阻力的量化显示了连续体行为的破坏。尖端速度和离表面距离的非单调依赖关系意味着，在比水团形成更小的时间尺度上，移动尖端周围的水化层被破坏，在最高速度下，水的可压缩性很强。
Structured water near surfaces is important in nonclassical crystallization, biomineralization, and restructuring of cellular membranes. In addition to equilibrium structures, studied by atomic force microscopy (AFM), high-speed AFM (H-S AFM) can now detect piconewton forces in microseconds. With increasing speeds and decreasing tip diameters, there is a danger that continuum water models will not hold, and molecular dynamic (MD) simulations would be needed for accurate predictions. MD simulations, however, can only evolve over tens of nanoseconds due to memory and computational efficiency/speed limitations, so new methods are needed to bridge the gap. Here, we report a hybrid, multiscale simulation method, which can bridge the size and time scale gaps to existing experiments. Structured water is studied between a moving silica AFM colloidal tip and a cleaved mica surface. The computational domain includes 1,472,766 atoms. To mimic the effect of long-range hydrodynamic forces occurring in water, when moving the AFM tip at speeds from 5 × 10–7 to 30 m/s, a hybrid multiscale method with local atomistic resolution is used, which serves as an effective open-domain boundary condition. The multiscale simulation is thus equivalent to using a macroscopically large computational domain with equilibrium boundary conditions. Quantification of the drag force shows the breaking of continuum behavior. Nonmonotonic dependence on both the tip speed and distance from the surface implies breaking of the hydration layer around the moving tip at time scales smaller than water cluster formation and strong water compressibility effects at the highest speeds.
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