Evaporation of Initially Heated Sessile Droplets and the Resultant Dried Colloidal Deposits on Substrates Held at Ambient Temperature.

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 are used as essential tools for interfacial temperature measurements and quantification of 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 toward 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 the fast decay of the temperature gradient, the coffee-ring dimensions significantly diminish, leading to an inner deposit. A reduction of 50-70% in the coffee-ring dimensions is recorded by elevating the initial droplet temperature from 25 to 75 °C for suspended particle concentration varying between 0.05 and 1.0% v/v. 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 evaporation, even after the interfacial temperature gradient vanishes. This is essentially a consequence of liquid inertia. Finally, a finite-element-based two-dimensional modeling in axisymmetric geometry is found to capture the measurements with reasonable fidelity and the hypothesis considered in the present study corroborates well with a first approximation qualitative scaling analysis. Overall, together with a new experimental condition, the present investigation discloses a distinct nature of Marangoni stress-induced flow in a drying droplet and its role in influencing the associated colloidal deposits, which was not explored previously. The insights gained from this study are useful to advance technical applications such as spray cooling, inkjet printing, bioassays, etc.