Using TIRF microscopy to quantify and confirm efficient mass transfer at the substrate surface of the chemistrode

This paper describes experiments for characterizing mass transfer at the hydrophilic surface of the substrate in a chemistrode. The chemistrode uses microfluidic plugs to deliver pulses of chemicals to a substrate with high temporal resolution, which requires efficient mass transfer between the wetting layer and the hydrophilic surface of the substrate. Here, total internal reflection fluorescence microscopy (TIRFM) was used to image the hydrophilic surface of the substrate as plugs were made to flow over it. The surface of the substrate was rapidly saturated with a fluorescent dye as the fluroesecent plugs passed over the substrate, confirming effective mass transfer between the wetting layer and the surface of the substrate. The dynamics of saturation are consistent from cycle to cycle, indicating that the chemistrode can stimulate surfaces with high reproducibility. The number of plugs required to reach 90% saturation of the hydrophilic surface of the substrate, ϕ(90%), only weakly depended on experimental conditions (the Péclet number or the capillary number). Furthermore, over a wide range of operating conditions, ϕ(90%) was less than 4. These results are useful for improving the chemistrode and for understanding other phenomena that involve diffusional transfer in multiphase or recirculating flows near surfaces.