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Register a new userThermal noise influences fluid flow in thin films during spinodal dewetting
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Experiments on dewetting thin polymer films confirm the theoretical prediction that thermal noise can strongly influence characteristic time-scales of fluid flow and cause coarsening of typical length scales. Comparing the experiments with deterministic simulations, we show that the Navier-Stokes equation has to be extended by a conserved bulk noise term to accomplish the observed spectrum of capillary waves. Due to thermal fluctuations the spectrum changes from an exponential to a power law decay for large wavevectors. Also the time evolution of the typical wavevector of unstable perturbations exhibits noise induced coarsening that is absent in deterministic hydrodynamic flow.
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The spontaneous formation of droplets via dewetting of a thin fluid film from a solid substrate allows for materials nanostructuring, under appropriate experimental control. While thermal fluctuations are expected to play a role in this process, their relevance has remained poorly understood, particularly during the nonlinear stages of evolution. Within a stochastic lubrication framework, we show that thermal noise speeds up and substantially influences the formation and evolution of the droplet arrangement. As compared with their deterministic counterparts, for a fixed spatial domain, stochastic systems feature a smaller number of droplets, with a larger variability in sizes and space distribution. Finally, we discuss the influence of stochasticity on droplet coarsening for very long times.
This study reveals the influence of the surface energy and solid/liquid boundary condition on the breakup mechanism of dewetting ultra-thin polymer films. Using silane self-assembled monolayers, SiO$_2$ substrates are rendered hydrophobic and provide a strong slip rather than a no-slip solid/liquid boundary condition. On undergoing these changes, the thin-film breakup morphology changes dramatically -- from a spinodal mechanism to a breakup which is governed by nucleation and growth. The experiments reveal a dependence of the hole density on film thickness and temperature. The combination of lowered surface energy and hydrodynamic slip brings the studied system closer to the conditions encountered in bursting unsupported films. As for unsupported polymer films, a critical nucleus size is inferred from a free energy model. This critical nucleus size is supported by the film breakup observed in the experiments using high speed emph{in situ} atomic force microscopy.
We study a model for a thin liquid film dewetting from a periodic heterogeneous substrate (template). The amplitude and periodicity of a striped template heterogeneity necessary to obtain a stable periodic stripe pattern, i.e. pinning, are computed. This requires a stabilization of the longitudinal and transversal modes driving the typical coarsening dynamics during dewetting of a thin film on a homogeneous substrate. If the heterogeneity has a larger spatial period than the critical dewetting mode, weak heterogeneities are sufficient for pinning. A large region of coexistence between coarsening dynamics and pinning is found.
We investigate the effect of short chains on slip of highly entangled polystyrenes (PS) during thin film dewetting from non-wetting fluorinated surfaces. Binary and ternary mixtures were prepared from monodisperse PS with weight average molecular weights $5 < M_textrm{w} < 490$ kg/mol. Flow dynamics and rim morphology of dewetting holes were captured using optical and atomic force microscopy. Slip properties are assessed in the framework of hydrodynamic models describing the rim height profile of dewetting holes. We show that short chains with $M_textrm{w}$ below the polymer critical molecular weight for entanglements, $M_textrm{c}$, can play an important role in slip of highly entangled polymers. Among mixtures of the same $M_textrm{w}$, those containing chains with $M<M_textrm{c}$ exhibit larger slip lengths as the number average molecular weight, $M_textrm{n}$, decreases. The slip enhancement effect is only applicable when chains with $M<M_textrm{c}$ are mixed with highly entangled chains such that the content of the long chain component, $phi_textrm{L}$, is dominant ($phi_textrm{L}<0.5$). These results suggest that short chains affect slip of highly entangled polymers on non-wetting surfaces due to the physical or chemical disparities of end groups, and any associated dynamical effect their presence may have, as compared to the backbone units. The enhanced slip in this regard is attributed to the impact of chain end groups or short chain enrichment on the effective interfacial friction coefficient. Accordingly, for entangled PS, a higher concentration of end groups or short chains at the interface results in a lower effective friction coefficient which consequently enhances the slip length.
We study the dewetting of liquid films capped by a thin elastomeric layer. When the tension in the elastomer is isotropic, circular holes grow at a rate which decreases with increasing tension. The morphology of holes and rim stability can be controlled by changing the boundary conditions and tension in the capping film. When the capping film is prepared with a biaxial tension, holes form with a non-circular shape elongated along the high tension axis. With suitable choice of elastic boundary conditions, samples can even be designed such that square holes appear.
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