Marangoni Droplets of Dextran in PEG Solution and Its Motile Change Due to Coil-Globule Transition of Coexisting DNA.

Motile droplets using Marangoni convection are attracting attention for their potential as cell-mimicking small robots. However, the motion of droplets relative to the internal and external environments that generate Marangoni convection has not been quantitatively described. In this study, we used an aqueous two-phase system [poly(ethylene glycol) (PEG) and dextran] in an elongated chamber to generate motile dextran droplets in a constant PEG concentration gradient. We demonstrated that dextran droplets move by Marangoni convection, resulting from the PEG concentration gradient and the active transport of PEG and dextran into and out of the motile dextran droplet. Furthermore, by spontaneously incorporating long DNA into the dextran droplets, we achieved cell-like motility changes controlled by coexisting environment-sensing molecules. The DNA changes its position within the droplet and motile speed in response to external conditions. In the presence of Mg2+, the coil-globule transition of DNA inside the droplet accelerates the motile speed due to the decrease in the droplet's dynamic viscosity. Globule DNA condenses at the rear part of the droplet along the convection, while coil DNA moves away from the droplet's central axis, separating the dipole convections. These results provide a blueprint for designing autonomous small robots using phase-separated droplets, which change the mobility and molecular distribution within the droplet in reaction with the environment. It will also open unexplored areas of self-assembly mechanisms through phase separation under convections, such as intracellular phase separation.

Cell-Sized Confinements Alter Molecular Diffusion in Concentrated Polymer Solutions Due to Length-Dependent Wetting of Polymers.

Living cells are characterized by the micrometric confinement of various macromolecules at high concentrations. Using droplets containing binary polymer blends as artificial cells, we previously showed that cell-sized confinement causes phase separation of the binary polymer solutions because of the length-dependent wetting of the polymers. Here, we demonstrate that the confinement-induced heterogeneity of polymers also emerges in single-component polymer solutions. The resulting structural heterogeneity also leads to a slower transport of small molecules at the center of cell-sized droplets than that in bulk solutions. Coarse-grained molecular simulations support this confinement-induced heterogeneous distribution by polymer length and demonstrate that the effective wetting of the shorter chains at the droplet surface originates from the length-dependent conformational entropy. Our results suggest that cell-sized confinement functions as a structural regulator for polydisperse polymer solutions that specifically manipulates the diffusion of molecules, particularly those with sizes close to the correlation length of the polymer chains.

Cross over to collective rearrangements near the dry-wet transition in two-dimensional foams.

Liquid foams respond plastically to external perturbations over some critical magnitude. This rearrangement process is directly related to the mechanical properties of the foams, playing a significant role in determining foam lifetime, deformability, elasticity, and fluidity. In this paper, we experimentally investigate the rearrangement dynamics of foams near a dry-wet transition. When a foam transforms from a dry state to a wet state, it is found that considering collective events, separated T1 events propagate in dry foams, while T1 events occur simultaneously in wet foams. This cross over to collective rearrangements is closely related to the change in local bubble arrangements and mobility. Furthermore, it is also found that a probability of collective rearrangement events occurring follows a Poisson distribution, suggesting that there is little correlation between discrete collective rearrangement events. These results constitute progress in understanding the dynamical properties of soft jammed systems, relevant for biological and material sciences as well as food science.

Dynamics and mechanism of liquid film collapse in a foam.

Foams have unique properties that distinguish them from ordinary liquids and gases, and are ubiquitously observed in nature, both in biological systems and industrial products. Foams are known to eventually collapse over time; given their wide-range industrial application, understanding how bubbles in a foam collapse is an important aspect for product longevity and tailoring physical properties. Previously, it was shown that droplets are emitted during the collective bubble collapse, however the mechanism of the droplet emission in a foam is not yet clearly understood. It is directly related to the stability of the foam, thus we quantitatively investigate collapse dynamics in liquid films in a foam, and identify some unique features. When one film breaks, we see that the oscillation of the vertical Plateau border to which it is connected induces anomalous liquid transport from the edge of the border to the center. Once a crack appears near the border and a collapse front is formed, we find that the curvature of the front reverses as it migrates, followed by the emergence and emission of droplets. We elucidate the origins of this behavior and discuss the stability of foams, establishing how the characteristic time scales of the process relate to each other.

Size distribution dependence of collective relaxation dynamics in a two-dimensional wet foam.

Foams can be ubiquitously observed in nature and in industrial products. Despite the relevance of their properties to deformation, fluidity, and collapse, all of which are essential for applications, there are few experimental studies of collective relaxation dynamics in a wet foam. Here, we directly observe how the relaxation dynamics changes with increasing liquid fraction in both monodisperse and polydisperse two-dimensional foams. As we increase the liquid fraction, we quantitatively characterize the slowing-down of the relaxation, and the increase of the correlation length. We also find two different relaxation modes which depend on the size distribution of the bubbles. It suggests that the bubbles which are simply near to each other play an important role in large rearrangements, not just those in direct contact. Finally, we confirm the generality of our experimental findings by a numerical simulation for the relaxation process of wet foams.

In-situ observation of collective bubble collapse dynamics in a quasi-two-dimensional foam.

The stability of foams is an important subject not only for fundamental science, but for applications in daily life. The most destructive phenomenon underpinning foam collapse is a collective bubble collapse, yet the mechanism behind this is unclear. In this study, we clarify the dynamics of the collective bubble collapse in a quasi-two-dimensional foam by in-situ observation with a high speed camera. We find two modes for collective bubble collapse: one is the propagation of liquid film breakage via impact with the stream of another broken liquid film. The other is breakage of a distant liquid film due to penetration by a liquid droplet, emitted by impact with the flow of a broken liquid film. As the liquid fraction increases, the velocity of liquid droplets decreases. Instead of penetration, the liquid droplet bounces like a billiard ball or it is absorbed into other films.

Dynamical transition in a jammed state of a quasi-two-dimensional foam.

The states of foam are empirically classified into dry foam and wet foam by the volume fraction of the liquid. Recently, a transition between the dry foam state and the wet foam state has been found by characterizing the bubble shapes [Furuta et al., Sci. Rep. 6, 37506 (2016)2045-232210.1038/srep37506]. In the literature, it is indirectly ascertained that the transition from the dry to the wet form is related to the onset of the rearrangement of the bubbles, namely, the liquid fraction at which the bubbles become able to move to replace their positions. The bubble shape is a static property, and the rearrangement of the bubbles is a dynamic property. Thus, we investigate the relation between the bubble shape transition and the rearrangement event occurring in a collapsing process of the bubbles in a quasi-two-dimensional foam system. The current setup brings a good advantage to observe the above transitions, since the liquid fraction of the foam continuously changes in the system. It is revealed that the rearrangement of the bubbles takes place at the dry-wet transition point where the characteristics of the bubble shape change.