Ring-shaped colloidal patterns on saline water films.

HYPOTHESIS: Electrostatically stabilised colloidal particles destabilise when brought into contact with cations causing the particles to aggregate in clusters. When a drop with stabilised colloidal partices is deposited on a liquid film containing cations the delicate balance between the fluid-mechanical and physicochemical properties of the system governs the spreading dynamics and formation of colloidal particle clusters. EXPERIMENTS: High-speed imaging and digital holographic microscopy were used to characterise the spreading process. FINDINGS: We reveal that a spreading colloidal drop evolves into a ring-shaped pattern after it is deposited on a thin saline water film. Clustered colloidal particles aggregate into larger trapezoidally-shaped 'supraclusters'. Using a simple model we show that the trapezoidal shape of the supraclusters is determined by the transition from inertial spreading dynamics to Marangoni flow. These results may be of interest to applications such as wet-on-wet inkjet printing, where particle destabilisation and hydrodynamic flow coexist.

Evaporating droplets on oil-wetted surfaces: Suppression of the coffee-stain effect.

The evaporation of suspension droplets is the underlying mechanism in many surface-coating and surface-patterning applications. However, the uniformity of the final deposit suffers from the coffee-stain effect caused by contact line pinning. Here, we show that control over particle deposition can be achieved through droplet evaporation on oil-wetted hydrophilic surfaces. We demonstrate by flow visualization, theory, and numerics that the final deposit of the particles is governed by the coupling of the flow field in the evaporating droplet, the movement of its contact line, and the wetting state of the thin film surrounding the droplet. We show that the dynamics of the contact line can be tuned through the addition of a surfactant, thereby controlling the surface energies, which then leads to control over the final particle deposit. We also obtain an analytical expression for the radial velocity profile which reflects the hindering of the evaporation at the rim of the droplet by the nonvolatile oil meniscus, preventing flow toward the contact line, thus suppressing the coffee-stain effect. Finally, we confirm our physical interpretation by numerical simulations that are in qualitative agreement with the experiment.

Evaporation-Induced Crystallization of Surfactants in Sessile Multicomponent Droplets.

Surfactants have been widely studied and used in controlling droplet evaporation. In this work, we observe and study the crystallization of sodium dodecyl sulfate (SDS) within an evaporating glycerol-water mixture droplet. The crystallization is induced by the preferential evaporation of water, which decreases the solubility of SDS in the mixture. As a consequence, the crystals shield the droplet surface and cease the evaporation. The universality of the evaporation characteristics for a range of droplet sizes is revealed by applying a diffusion model, extended by Raoult's law. To describe the nucleation and growth of the crystals, we employ the 2-dimensional crystallization model of Weinberg [J. Non-Cryst. Solids 1991, 134, 116]. The results of this model compare favorably to our experimental results. Our findings may inspire the community to reconsider the role of high concentration of surfactants in a multicomponent evaporation system.

Systematic approach for wettability prediction using molecular dynamics simulations.

We present a fast and efficient approach to predict the wettability and spreading of liquids on polymeric substrates. First, a molecular dynamics parameterization is proposed for the calculation of the solubility parameter for 74 compounds including surfactants typically used in inkjet printing. Then, we introduce a molecular geometrical factor to relate the solubility parameter to the surface tension, obtaining estimates in remarkable agreement with experiments. By using a modified Young-Fowkes equation, the contact angles of liquids on various polymeric substrates are determined and their dependence on the hydrogen bonding, dispersion and polar contribution of the solubility parameter are investigated. We find that wetting properties are obtained with a good accuracy when taking into account the hydrogen-bonding and polar interactions in the geometric sum of the solubility parameter. Based on these findings, a 3D wetting space is proposed to evaluate liquids wettability and judge their suitability for specific substrates. This will enable easy formulation of liquids with wettability tailored for a particular surface and application.

Gravitational Effect in Evaporating Binary Microdroplets.

The flow in an evaporating glycerol-water binary submillimeter droplet with a Bond number Bo≪1 is studied both experimentally and numerically. First, we measure the flow fields near the substrate by microparticle image velocimetry for both sessile and pendant droplets during the evaporation process, which surprisingly show opposite radial flow directions-inward and outward, respectively. This observation clearly reveals that in spite of the small droplet size, gravitational effects play a crucial role in controlling the flow fields in the evaporating droplets. We theoretically analyze that this gravity-driven effect is triggered by the lower volatility of glycerol which leads to a preferential evaporation of water then the local concentration difference of the two components leads to a density gradient that drives the convective flow. We show that the Archimedes number Ar is the nondimensional control parameter for the occurrence of the gravitational effects. We confirm our hypothesis by experimentally comparing two evaporating microdroplet systems, namely, a glycerol-water droplet and a 1,2-propanediol-water droplet. We obtain different Ar, larger or smaller than a unit by varying a series of droplet heights, which corresponds to cases with or without gravitational effects, respectively. Finally, we simulate the process numerically, finding good agreement with the experimental results and again confirming our interpretation.

Evaporation-Triggered Segregation of Sessile Binary Droplets.

Droplet evaporation of multicomponent droplets is essential for various physiochemical applications, e.g., in inkjet printing, spray cooling, and microfabrication. In this work, we observe and study the phase segregation of an evaporating sessile binary droplet, consisting of a miscible mixture of water and a surfactantlike liquid (1,2-hexanediol). The phase segregation (i.e., demixing) leads to a reduced water evaporation rate of the droplet, and eventually the evaporation process ceases due to shielding of the water by the nonvolatile 1,2-hexanediol. Visualizations of the flow field by particle image velocimetry and numerical simulations reveal that the timescale of water evaporation at the droplet rim is faster than that of the Marangoni flow, which originates from the surface tension difference between water and 1,2-hexanediol, eventually leading to segregation.

Regimes of bubble volume oscillations in a pipe.

The effect of an acoustically driven bubble on the acoustics of a liquid-filled pipe is theoretically analyzed and the dimensionless groups of the problem are identified. The different regimes of bubble volume oscillations are predicted theoretically with these dimensionless groups. Three main regimes can be identified: (1) For small bubbles and weak driving, the effect of the bubble oscillations on the acoustic field can be neglected. (2) For larger bubbles and still small driving, the bubble affects the acoustic field, but due to the small driving, a linear theory is sufficient. (3) For large bubbles and large driving, the two-way coupling between the bubble and the flow dynamics requires the solution of the full nonlinear problem. The developed theory is then applied to an air bubble in a channel of an inkjet printhead. A numerical model is developed to test the predictions of the theoretical analysis. The Rayleigh-Plesset equation is extended to include the influence of the bubble volume oscillations on the acoustic field and vice versa. This modified Rayleigh-Plesset equation is coupled to a channel acoustics calculation and a Navier-Stokes solver for the flow in the nozzle. The numerical simulations indeed confirm the predictions of the theoretical analysis.

Acoustic measurement of bubble size in an inkjet printhead.

The volume of a bubble in a piezoinkjet printhead is measured acoustically. The method is based on a numerical model of the investigated system. The piezo not only drives the system but it is also used as a sensor by measuring the current it generates. The numerical model is used to predict this current for a given bubble volume. The inverse problem is to infer the bubble volume from an experimentally obtained piezocurrent. By solving this inverse problem, the size and position of the bubble can thus be measured acoustically. The method is experimentally validated with an inkjet printhead that is augmented with a glass connection channel, through which the bubble was observed optically, while at the same time the piezocurrent was measured. The results from the acoustical measurement method correspond closely to the results from the optical measurement.

Effect of an entrained air bubble on the acoustics of an ink channel.

Piezo-driven inkjet systems are very sensitive to air entrapment. The entrapped air bubbles grow by rectified diffusion in the ink channel and finally result in nozzle failure. Experimental results on the dynamics of fully grown air bubbles are presented. It is found that the bubble counteracts the pressure buildup necessary for the droplet formation. The channel acoustics and the air bubble dynamics are modeled. For good agreement with the experimental data it is crucial to include the confined geometry into the model: The air bubble acts back on the acoustic field in the channel and thus on its own dynamics. This two-way coupling limits further bubble growth and thus determines the saturation size of the bubble.