The present study experimentally and numerically investigates the evaporation and resultant patterns of dried deposits of aqueous colloidal sessile droplets, when the droplets are initially elevated to a high temperature before being placed on a substrate held at ambient temperature. The system is then released for natural evaporation without applying any external perturbation. Infrared thermography and optical profilometry were used as essential tools for interfacial temperature measurements and quantification of the coffee-ring dimensions, respectively. Initially, a significant temperature gradient exists along the liquid-gas interface as soon as the droplet is deposited on the substrate which triggers a Marangoni stress-induced recirculation flow directed from the top of the droplet towards the contact line along the liquid-gas interface. Thus, the flow is in the reverse direction to that seen in the conventional substrate heating case. Interestingly, this temperature gradient decays rapidly -- within the first 10% of the total evaporation time and the droplet-substrate system reaches thermal equilibrium with ambient thereafter. Despite fast decay of the temperature gradient, the coffee-ring dimensions significantly diminish, leading to an inner deposit. This suppression of the coffee-ring effect is attributed to the fact that the initial Marangoni stress-induced recirculation flow continues until the last stage of the evaporation, even after the interfacial temperature gradient vanishes. This is essentially a consequence of liquid inertia. Overall, together with a new experimental condition, the present investigation discloses a distinct nature of Marangoni stress-induced flow in the drying droplet and its role in influencing the associated colloidal deposits, which was not explored previously.
Understanding flow patterns and coupled transport phenomena during evaporation of droplets loaded with colloidal particles is central to design technical applications such as organizing proteins/DNA on a solid surface. We review recent reports on evaporating sessile droplets of colloidal suspensions on a solid surface. Starting from the classical mechanism of formation of a ring-like deposit, we discuss the influence of several problem parameters. Notably, thermal or solutal Marangoni effect, particle size, particle concentration, particle shape, substrate wettability, pH of the suspension etc…
Effects of substrate temperature, substrate wettability and particles concentration are experimentally investigated for evaporation of a sessile water droplet containing colloidal particles. Time-varying droplet shapes and temperature of the liquid-gas interface are measured using high-speed visualization and infrared thermography, respectively. The motion of the particles inside the evaporating droplet is qualitatively visualized by an optical microscope and profile of final particle deposit is measured by an optical profilometer. On a non-heated hydrophilic substrate, a ring-like deposit for…
We experimentally investigate the profile and morphology of the ring-like deposits obtained after evaporation of a sessile water droplet containing polystyrene colloidal particles on a hydrophilic glass substrate. In particular, the coupled effect of particle size and concentration are studied. The deposits were qualitatively visualized under an optical microscope and profile of the ring was measured by an optical profilometer. The profile of the ring resembles a partial torus-like shape for all cases of particles size and concentration. The cracks on the surface of the ring were found to occu…
We investigate deposit patterns and associated morphology formed after the evaporation of an aqueous droplet containing mono- and bi-dispersed colloidal particles. In particular, the combined effect of substrate heating and particle diameter is investigated. We employ high-speed visualization, optical microscopy and scanning electron microscopy to characterize the evaporating droplets, particle motion, and deposit morphology, respectively. In the context of mono-dispersed colloidal particles, an inner deposit and a typical ring form for smaller and larger particles, respectively, on a nonheate…
The so-called coffee stain effect has been intensively studied over the past decades, but most of the studies are focused on sessile droplets. In this paper, we analyse the origin of the difference between the deposition of suspended particles in a sessile drop and in an axisymmetric drop deposited on a fibre. First, we model the shape of a drop on a fibre and its evaporative flux with some approximations to derive analytical calculations. Then, for pinned contact lines, we solve the hydrodynamics equations in the liquid phase under the lubrication approximation to determine the flow velocity …
The investigation of evaporating liquid drop deposited onto a flat surface is of great importance for physical, engineering and medical applications. Novel analytical expressions are proposed to calculate the evaporation rate of sessile drop (mass loss per unit surface area per unit time) and total evaporation rate (mass loss per unit time). To obtain these results, the H.M. Macdonald's solution for a flat wedge was transformed by method of inversion in a sphere originally developed by J.C. Maxwell in the Treatise on Electricity and Magnetism with further derivation the solution for a lens bas…
Spreading of respiratory diseases, such as COVID-19, from contaminated surfaces is dependent on the drying time of the deposited droplets containing the virus. The evaporation rate depends on environmental conditions, such as ambient temperature and relative humidity and physical properties (e.g., droplet volume, contact angle and composition). The respiratory droplets contain salt (NaCl), protein (mucin), and surfactant (dipalmitoylphosphatidylcholine) in addition to water, which are expected to influence the evaporation in a big way. A diffusion-based theoretical model for estimating the dry…
The evaporation of a sessile droplet spontaneously induces an internal capillary liquid flow. The surface-tension driven minimisation of surface area and/or surface-tension differences at the liquid-gas interface caused by evaporation-induced temperature or chemical gradients set the liquid into motion. This flow drags along suspended material and is one of the keys to control the material deposition in the stain that is left behind by a drying droplet. Applications of this principle range from the control of stain formation in the printing and coating industry, to the analysis of DNA, to fore…
We propose a theory for the multi-ring pattern of the deposits that are formed when droplets of suspension are dried on a substrate. Assuming a standard model for the stick-slip motion of the contact line, we show that as droplets evaporate, many concentric rings of deposits are formed, but are taken over by a solid-circle pattern in the final stage of drying. An analytical expression is given to indicate when ring-pattern changes to solid-circle pattern during an evaporation process. The results are in qualitative agreement with existing experiments, and the other predictions on how the evapo…
Coalescence-induced alignment of anisotropic particles in drying sessile droplets
Forschungszentrum Jülich（于利希研究中心）；Helmholtz Institute Erlangen-Nürnberg for Renewable Energy (IET-2)（亥姆霍兹埃尔朗根-纽伦堡可再生能源研究所（IET-2））；Friedrich-Alexander-Universität Erlangen-Nürnberg（埃尔朗根-纽伦堡弗里德里希·亚历山大大学）
We study the effects of vertical sinusoidal vibrations on a liquid droplet with a low surface tension (ethanol) deposited on a solid substrate. In a precise range of amplitudes and frequencies, the drop exhibits a dramatic worm-like shape instability with a strong symmetry breaking, comparable to the one observed by Pucci et al. (Phys. Rev. Lett., 106 (2011) 024503) on a vibrated floating lens. However, the geometry of our system is much simpler since it does not involve the oscillation and deformation of a liquid-liquid-air contact line. We show that the Faraday waves appearing on the surface…
We study the size and shape of the final deposit obtained when a drop with colloidal particles has dried on a super-hydrophobic surface made of micro-posts. As expected, most of the particles lie inside a circular area, which radius roughly corresponds to the Laplace pressure threshold for liquid impalement inside the structure (Cassie-Wenzel transition), inducing a coffee-stain deposit due to contact-line pinning. Less expected is the observation of tiny deposits on top of posts in the area external to the main ring, despite the low macroscopic liquid/solid friction. Experiments are carried o…
The deposition of particles on a surface by an evaporating sessile droplet is important for phenomena as diverse as printing, thin-film deposition and self-assembly. The shape of the final deposit depends on the flows within the droplet during evaporation. These flows are typically determined at the onset of the process by the intrinsic physical, chemical and geometrical properties of the droplet and its environment. Here, we demonstrate deterministic emergence and real-time control of Marangoni flows within the evaporating droplet by an external point-source of vapor. By varying the source lo…
Building on the recent theoretical work of Wray, Duffy and Wilson [J. Fluid Mech. 884, A45 (2020)] concerning the competitive diffusion-limited evaporation of multiple thin sessile droplets in proximity to each other, we obtain theoretical predictions for the spatially non-uniform densities of the contact-line deposits (often referred to as "coffee stains" or "ring stains") left on the substrate after such droplets containing suspended solid particles have completely evaporated. Neighbouring droplets interact via their vapour fields, which results in a spatially non-uniform "shielding" effect.…
The internal dynamics during the coalescence of a sessile droplet and a subsequently deposited impacting droplet, with either identical or distinct surface tension, is studied experimentally in the regime where surface tension is dominant. Two color high-speed cameras are used to capture the rapid internal flows and associated mixing from both side and bottom views simultaneously by adding an inert dye to the impacting droplet. Given sufficient lateral separation between droplets of identical surface tension, a robust surface jet is identified on top of the coalesced droplet. Image processing …
This paper presents an experimental study on thermal transport to single water droplets evaporating on heated bi-phobic surfaces consisting of a superhydrophobic matrix with a circular hydrophobic pattern with strong contact line pinning. A single water droplet of 8 ul volume is placed on a preheated surface and allowed to evaporate in an open laboratory environment. We investigate the influence of substrate orientation (horizontal and vertical) on evaporation dynamics. Using optical and infrared imaging, we report droplet fluid dynamics and heat transfer characteristics of the evaporating dro…
Hypothesis: Contact-line motion upon drying of sessile droplet strongly affects the solute transport and solvent evaporation profile. Hence, it should have a strong impact on the deposit formation and might be responsible for volcano-like, dome-like and at deposit morphologies. Experiments: A method based on a thin-film interference was used to track the drop height profile and contact line motion during the drying. A diverse set of drying scenarios was obtained by using inks with different solvent compositions and by adjusting the substrate wetting properties. The experimental data was compar…
When a colloidal sessile droplet dries on a substrate, the particles suspended in it usually deposit in a ring-like pattern. This phenomenon is commonly referred to as the "coffee-ring" effect. One paradigm for why this occurs is as a consequence of the solutes being transported towards the pinned contact line by the flow inside the drop, which is induced by surface evaporation. From this perspective, the role of the liquid-gas interface in shaping the deposition pattern is somewhat minimized. Here, we propose an alternative mechanism for the coffee-ring deposition. It is based on the bulk flo…
The shape of deposits obtained from drying drops containing colloidal particles matters for technologies such as inkjet printing, microelectronics and bioassay manufacturing. In this work, the formation of deposits during the drying of nanoliter drops containing colloidal particles is investigated experimentally with microscopy and profilometry, and theoretically with an inhouse finite-element code. The system studied involves aqueous drops containing titania nanoparticles evaporating on a glass substrate. Deposit shapes from spotted drops at different pH values are measured using a laser prof…
An efficient way to precisely pattern particles on solid surfaces is to dispense and evaporate colloidal drops, as for bioassays. The dried deposits often exhibit complex structures exemplified by the coffee ring pattern, where most particles have accumulated at the periphery of the deposit. In this work, the formation of deposits during the drying of nanoliter colloidal drops on a flat substrate is investigated numerically and experimentally. A finite-element numerical model is developed that solves the Navier-Stokes, heat and mass transport equations in a Lagrangian framework. The diffusion …
We experimentally investigate the evaporation characteristics of a sessile ethanol droplet containing Al$_2$O$_3$ and Cu nanoparticles of sizes 25 nm and 75 nm on a heated substrate using shadowgraphy and infrared imaging techniques. Our results demonstrate that the droplet contact line dynamics resulting from the presence of various nanoparticles plays a dominant role in the evaporation process. This is in contrast to the widely-held assumption that the enhanced evaporation rate observed in sessile nanofluid droplets is due to the higher thermal conductivity of the added nanoparticles. We obs…
Evaporating liquid droplets are omnipresent in nature and technology, such as in inkjet printing, coating, deposition of materials, medical diagnostics, agriculture, food industry, cosmetics, or spills of liquids. While the evaporation of pure liquids, liquids with dispersed particles, or even liquid mixtures has intensively been studied over the last two decades, the evaporation of ternary mixtures of liquids with different volatilities and mutual solubilities has not yet been explored. Here we show that the evaporation of such ternary mixtures can trigger a phase transition and the nucleatio…
