In molecular-level fluidic transport, where the discrete characteristics of a molecular system are not negligible (in contrast to a continuum description), the response of the molecular water system might still be similar to the continuum description if the time and ensemble averages satisfy the ergodic hypothesis and the scale of the average is enough to recover the classical thermodynamic properties. However, even in such cases, the continuum description breaks down on the material interfaces. In short, molecular-level liquid flows exhibit substantially different physics from classical fluid transport theories because of (i) the interface/surface force field, (ii) thermal/velocity slip, (iii) the discreteness of fluid molecules at the interface and (iv) local viscosity. Therefore, in this study, we present the result of our investigations using molecular dynamics (MD) simulations with continuum-based energy equations and check the validity and limitations of the continuum hypothesis. Our study shows that when the continuum description is subjected to the proper treatment of the interface effects via modified boundary conditions, the so-called continuum-based modified-analytical solutions, they can adequately predict nanoscale fluid transport phenomena. The findings in this work have broad effects in overcoming current limitations in modeling/predicting the fluid behaviors of molecular fluidic devices.
In this paper, we present an approach for predicting nanoscale capillary imbibitions using the Lucas-Washburn (LW) theory. Molecular dynamics (MD) simulations were employed to investigate the effects of surface forces on the viscosity of liquid water. This provides an update to the modified LW equation that considered only a nanoscale slip length. An initial water nanodroplet study was performed to properly elucidate the wetting behavior of copper and gold surfaces. Intermolecular interaction strengths between water and corresponding solid surfaces were determined by matching the contact angle values obtained by experimental measurements. The migration of liquid water into copper and gold capillaries was measured by MD simulations and was found to differ from the modified LW equation. We found that the liquid layering in the vicinity of the solid surface induces a higher density and viscosity, leading to a slower MD uptake of fluid into the capillaries than was theoretically predicted. The near-surface viscosity for the nanoscale-confined water was defined and calculated for the thin film of water that was sheared between the two solid surfaces, as the ratio of water shear stress to the applied shear rate. Considering the effects of both the interface viscosity and slip length of the fluid, we successfully predicted the MD-measured fluid rise in the nanotubes.
At the interface between monolayer coated solid substrate and fluid, the effect of interfacial mismatch on Kapitza length due to the monolayer particles has been extensively analyzed through a series of non-equilibrium molecular dynamics simulation.
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