Surfactant-Mediated Collapse of Liquid Marbles and Directed Assembly of Particles at the Liquid Surface

Langmuir. 2019 Apr 2;35(13):4566-4576. doi: 10.1021/acs.langmuir.8b03821. Epub 2019 Mar 14.

Abstract

Extensive research is being devoted to both the fundamental and applied aspects of liquid marbles (LMs). However, influence of the surface tension of the liquid substrate on the stability of the LMs and LM-mediated capillary interaction remains unexplored. In this work, we unveil the role of the surface tension of the liquid substrate on the collapse of multilayered LMs and apply this knowledge for realizing a dense planar assembly of microparticles triggered by LM-mediated capillary interactions. Experiments and analysis show that the required surface tension for the collapse is dependent on the volume of the LMs. The larger LMs are less stable, and thus collapse at a higher surface tension than that required for smaller LMs. The results are explained on the basis of the balance between surface tension forces acting on the LM ( Fs) and its weight ( Fw). Force analysis reveals that the collapse of the LM on the liquid substrate occurs when the surface tension force approaches to its weight, that is, when Fs ≈ Fw. This has been verified for LMs having volume in the range 6-10 μL. The experiments with different surfactants (an anionic and a cationic) lead to similar results which indicate that the collapse condition of the LMs is mainly dependent on their weight and the surface tension of the liquid substrate. Further, we demonstrate the LM-mediated assembly of particles at the liquid surface, and interestingly, the LM can be collapsed once the assembly is completed, leading to a denser well-packed assembled structure. We believe that the presented results could provide new insights in the fields of microfluidics, particle patterning, and assembly.