Initial solidification dynamics of spreading droplets

When a droplet is brought in contact with an undercooled surface, it wets the substrate and solidifies at the same time. The interplay between the phase transition effects and the contact-line motion, leading to its arrest, remains poorly understood. Here we reveal the early solidification patterns and dynamics of spreading hexadecane droplets. Total internal reflection imaging is employed to temporally and spatially resolve the early solidification behavior. With this, we determine the conditions leading to the contact-line arrest. We quantify the overall nucleation behavior, i.e., the nucleation rate and the crystal growth speed and show its sensitivity to the applied undercooling of the substrate. We also show that for strong enough undercooling it is the rapid growth of the crystals which determines the eventual arrest of the spreading contact line. By combining the Johnson-Mehl-Avrami-Kolmogorov nucleation theory and scaling relations for the spreading, we calculate the temporal evolution of the solid area fraction, which is in good agreement with our observations.