Real-time three-dimensional micro-imaging of liquid front in spreading sessile droplet under transient spreading states.

Dynamic wetting behaviors of sessile droplets on substrates play crucial roles for various industrial chemical processes. In the case of complete wetting, it has been proposed that a precursor film which is nanometer-order thickness and micrometer-order length further expands outside the macroscopic contact line of the sessile droplet. While the time evolution of the precursor film is believed to strikingly affect the macroscopic wetting behavior (e.g., spreading velocity), it had been hard to visualize the three-dimensional shape of the precursor film at the early stage of wetting. Further, although the spreading velocity rapidly decreases upon time at the early stage of the wetting (transient state) and then converged to be a constant at later time (steady state), conventional fluid mechanics theories generally describe only the wetting behavior at the steady state. Therefore, experimental observation of time evolution of the precursor film shape in the transient state is essential to proceed the theories to the next step. Here, a monochromatic laser interference microscope was developed to visualize three-dimensional shape of the wetting front of sessile droplets in real time. By detecting an interference of the laser reflected at the liquid and substrate surfaces, the precursor film was successfully visualized with a time resolution of 20 ms and a thickness resolution of about 3.5 nm at worst. For 10 cSt silicone oil on Si substrate, a 60-nm-thick and 70-μm-long precursor film was observed for 2-10 min after dropping and its spreading velocity which decreased with time was quantitatively analyzed.