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Sessile water droplets containing nano-silica particles are allowed to evaporate in the presence of driven substrate oscillations at chosen frequencies. Different mode shapes are observed at different oscillation frequencies. As reference, the evaporation of the same droplets is also observed under stationary conditions i.e. in the absence of any oscillations. For all cases, the deposit structures formed by the agglomeration of the nano-silica particles have been imaged. It has been observed that for the stationary droplets and for droplets whose oscillations are initiated close to the resonance of the lowest allowable oscillation mode, the structures are similar having larger spread over height, while for higher frequencies the structures are dome-like with more uniform outer dimensions. The possible reasons behind these structures are investigated using experimental techniques such as high-speed imaging of droplet oscillations, internal flow visualization and SEM imaging. Understanding of the underlying mechanisms behind the formation of these striking features is required for these methods to be applicable in larger scale drying operations or micro-device applications. Altogether a novel methodology has been presented and investigated for manipulating the morphological features in evaporating nano-particle laden sessile droplets.

We report the dynamics and underlying physics of evaporation driven transitions and autotuning of oscillation modes in sessile droplets subject to substrate perturbations. We have shown that evaporation controls temporal transition of the oscillation mode with a spatially downward shift of nodes (surface locations with zero displacement) toward the three-phase contact line. We have explained the physical mechanism using two parameters: the first quantifies evaporation driven tuning for resonance detection, and the second parameter characterizes mode lifetime which is found to be governed by evaporation dynamics. It is desirable to achieve autotuning of the oscillation modes in sessile droplets that essentially self-evolves in a spatiotemporal manner with continued evaporation. The insights suggest control of mode resonances is possible, which in turn will allow precision manipulations at droplet scale crucial for many applications such as surface patterning and others.

This work analyses the unique spatio-temporal alteration of the deposition pattern of evaporating nanoparticle laden droplets resting on a hydrophobic surface through targeted low frequency substrate vibrations. External excitation near the lowest resonant mode (n = 2) of the droplet initially de-pins and then subsequently re-pins the droplet edge creating pseudo-hydrophilicity (low contact angle). Vibration subsequently induces droplet shape oscillations (cyclic elongation and flattening) resulting in strong flow recirculation. This strong radially outward liquid flow augments nanoparticle transport, vaporization, and agglomeration near the pinned edge resulting in much reduced drying time under certain characteristic frequency of oscillations. The resultant deposit exhibits a much flatter structure with sharp, defined peripheral wedge topology as compared to natural drying. Such controlled manipulation of transport enables tailoring of structural and topological morphology of the deposits and offers possible routes towards controlling the formation and drying timescales which are crucial for applications ranging from pharmaceutics to surface patterning.

Evaporating sessile functional droplets act as the fundamental building block that controls the cumulative outcome of many industrial and biological applications such as surface patterning, 3D printing, photonic crystals, and DNA sequencing, to name a few. Additionally, a drying single sessile droplet forms a high-throughput processing technique using low material volume which is especially suitable for medical diagnosis. A sessile droplet also provides an elementary platform to study and analyze fundamental interfacial processes at various length scales ranging from macroscopically observable wetting and evaporation to microfluidic transport to interparticle forces operating at a nanometric length scale. As an example, to ascertain the quality of 3D printing we must understand the fundamental interfacial processes at the droplet scale. In this article, we review the coupled physics of evaporation flow-contact-line-driven particle transport in sessile colloidal droplets and provide methodologies to control the same. Through natural alterations in droplet vaporization, one can change the evaporative pattern and contact line dynamics leading to internal flow which will modulate the final particle assembly in a nontrivial fashion. We further show that control over particle transport can also be exerted by external stimuli which can be thermal, mechanical oscillations, vapor confinement (walled or a fellow droplet), or chemical (surfactant-induced) in nature. For example, significant augmentation of an otherwise evaporation-driven particle transport in sessile droplets can be brought about simply through controlled interfacial oscillations. The ability to control the final morphologies by manipulating the governing interfacial mechanisms in the precursor stages of droplet drying makes it perfectly suitable for fabrication-, mixing-, and diagnostic-based applications.

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Stacking pure solvent droplets on a solid substrate is apparently impossible in the absence of an external force as the second droplet will invariably spill over the first leading to a large wetted area. However, the unique feature that emerges during the drying of a nanoparticle laden droplet is the progressively enlarging thin solid film along the evaporating sessile droplet liquid periphery. This solid interface: the edge of which we shall refer to as the agglomeration front comprises of a thin layer of nanoparticle assembly and can support a carefully dispensed second droplet thereby allowing droplet stacking. It will be shown that the growth of this agglomeration front can also be effectively controlled by the dispensing time difference and the nanoparticle concentration in the two droplets. So far, we are commonly aware of material stacking in solid phase. This letter demonstrates stacking in the liquid phase and control over the thin solid interface growth.